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Biological materials and organisms possess the fundamental ability to self-organize, through which different components are assembled from the molecular level up to hierarchical structures with superior mechanical properties and multifunctionalities. These complex composites inspire material scientists to design new engineered materials by integrating multiple ingredients and structures over a wide range. Additive manufacturing, also known as 3D printing, has advantages with respect to fabricating multiscale and multi-material structures. The need for multifunctional materials is driving 3D printing techniques toward arbitrary 3D architectures with the next level of complexity. In this paper, the aim is to highlight key features of those 3D printing techniques that can produce either multiscale or multimaterial structures, including innovations in printing methods, materials processing approaches, and hardware improvements. Several issues and challenges related to current methods are discussed. Ultimately, the authors also provide their perspective on how to realize the combination of multiscale and multimaterial capabilities in 3D printing processes and future directions based on emerging research.

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Gelatin Methacryloyl (GelMA) is one of the most used biomaterials for a wide range of applications, such as drug delivery, disease modeling and tissue regeneration. GelMA is obtained from gelatin, which can be derived from different sources (e.g., bovine skin, and porcine skin), through substitution of reactive amine and hydroxyl groups with methacrylic anhydride (MAA). The degree of functionalization (DoF) can be tuned by varying the MAA amount used; thus, different protocols, with different reaction efficiency, have been developed, using various alkaline buffers (e.g., phosphate-buffered saline, DPBS, or carbonate-bicarbonate solution). Obviously, DoF modulation has an impact on the final GelMA properties, so a deep investigation on the features of the obtained hydrogel must be carried on. The purpose of this study is to investigate how different gelatin sources and synthesis methods affect GelMA properties, as literature lacks direct and systematic comparisons between these parameters, especially between synthesis methods. The final aim is to facilitate the choice of the source or synthesis method according to the needs of the desired application. Hence, chemical and physical properties of GelMA formulations were assessed, determining the DoFs, mechanical and viscoelastic properties by rheological analysis, water absorption by swelling capacity and enzymatic degradation rates. Biological tests with lung adenocarcinoma cells (A549) were performed. Moreover, since 3D bioprinting is a rapidly evolving technology thanks to the possibility of precise deposition of cell-laden biomaterials (bioinks) to mimic the 3D structures of several tissues, the potential of different GelMA formulations as bioinks have been tested with a multi-material approach, revealing its printability and versatility in various applications.

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This article presents the design and fabrication of a variable stiffness soft gripper based on layer jamming. Traditional layer jamming units have some limitations, such as complicated multistep fabrication, difficulties in system integration, and diminishing in stiffen effect. In this article, a variable stiffness soft gripper is proposed based on the rotational jamming layers to reduce the slippery phenomenon between layers. To fabricate the proposed complex design, a two-step fabrication method is presented. First, multimaterial 3D printing is applied to directly print out the soft finger body with jamming layers. Second, mold casting is used to fabricate the outer vacuum chamber. The proposed gripper contains a main framework and three identical variable stiffness soft fingers. To demonstrate the effectiveness of the design, the soft gripper is mounted on a robotic arm to test its ability of grasping heavy objects while following complex grasping trajectory. The gripper can successfully grasp an object up to 360 g. Grasping robustness of the proposed gripper can be guaranteed when the robotic arm is moving at acceleration up to 7 m/s2. The results prove that the proposed design of the soft gripper can improve the grippers grasping robustness during high-speed movement.

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Additive manufacturing, commonly known as 3D printing, allows decentralized drug fabrication of orally administered tablets. Microneedles are comparatively favorable for self-administered transdermal drug delivery with improved absorption and bioavailability. Due to the cross-scale geometric characteristics, 3D-printed microneedles face a significant trade-off between the feature resolution and production speed in conventional layer-wise deposition sequences. In this study, we introduce an economical and scalable direct ink drawing strategy to create drug-loaded microneedles. A freestanding microneedle is efficiently generated upon each pneumatic extrusion and controlled drawing process. Sharp tips of ∼5 µm are formed with submillimeter nozzles, representing 2 orders of magnitude improved resolution. As the key enabler of this fabrication strategy, the yield-stress fluid inks are formulated by simply filling silica nanoparticles into regular polymer solutions. The approach is compatible with various microneedles based on dissolvable, biodegradable, and nondegradable polymers. Various matrices are readily adopted to adjust the release behaviors of the drug-loaded microneedles. Successful fabrication of multifunctional patches with heterogeneously integrated microneedles allows the treatment of melanoma via synergistic photothermal therapy and combination chemotherapy. The personalized patches are designed for cancer severity to achieve high therapeutic efficacy with minimal side effects. The direct ink drawing reported here provides a facile and low-cost fabrication strategy for multifunctional microneedle patches for self-administering transdermal drug delivery.

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3D printing of multimaterial objects is an emerging field with promising applications. The layer-by-layer material addition technique used in 3D printing enables incorporation of distinct functionalized materials into the specialized devices. However, very few studies have been performed on the usage of multimaterial 3D printing for printable photonic and wearable devices. Here, we employ vat photopolymerization-based 3D printing to produce multimaterial contact lenses, offering enhanced multiband optical filtration, which can be valuable for tackling ocular conditions such as color blindness. A combination of hydroxyethyl methacrylate (HEMA) and polyethylene glycol diacrylate (PEGDA) was used as the base hydrogel for 3D printing. Atto565 and Atto488 dyes were added to the hydrogel for wavelength filtering, each dye suitable for a different type of color blindness. Multimaterial disks and contact lenses, with separate sections containing distinct dyes, were 3D-printed, and their optical properties were studied. The characteristics of multimaterial printing were analyzed, focusing on the formation of a uniform multimaterial interface. In addition, a novel technique was developed for printing multiple dyed materials in complex lateral geometrical patterns, by employing suitable variations in CAD models and the UV curing time. It was observed that the multimaterial printing process does not negatively affect the optical properties of the contact lenses. The printed multimaterial contact lenses offered a combined multi-band color blindness correction due to the two dyes used. The resulting optical spectrum was a close match to the commercially available color blindness correction glasses.

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Ionic conductive elastomers (ICEs) are emerging stretchable and ionic conductive materials that are solvent-free and thus demonstrate excellent thermal stability. Three-dimensional (3D) printing that creates complex 3D structures in free forms is considered as an ideal approach to manufacture sophisticated ICE-based devices. However, the current technologies constrain 3D printed ICE structures in a single material, which greatly limits functionality and performance of ICE-based devices and machines. Here, we report a digital light processing (DLP)-based multimaterial 3D printing capability to seemly integrate ultraviolet-curable ICE (UV-ICE) with nonconductive materials to create ionic flexible electronic devices in 3D forms with enhanced performance. This unique capability allows us to readily manufacture various 3D flexible electronic devices. To demonstrate this, we printed UV-ICE circuits into polymer substrates with different mechanical properties to create resistive strain and force sensors; we printed flexible capacitive sensors with high sensitivity (2 kPa-1) and a wide range of measured pressures (from 5 Pa to 550 kPa) by creating a complex microstructure in the dielectric layer; we even realized ionic conductor-activated four-dimensional (4D) printing by printing a UV-ICE circuit into a shape memory polymer substrate. The proposed approach paves a new efficient way to realize multifunctional flexible devices and machines by bonding ICEs with other polymers in 3D forms.

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Constructing precise metal patterns on complex three-dimensional (3D) plastic parts allows the fabrication of functional devices for advanced applications. However, it is currently expensive and requires complex processes. This study demonstrates a process for the fabrication of 3D metal-plastic composite structures with arbitrarily complex shapes. A light-cured resin is modified to prepare the active precursor allowing subsequent electroless plating (ELP). A multimaterial digital light processing 3D printer was newly developed to fabricate the parts containing regions made of either standard resin or active precursor nested within each other. Selective 3D ELP processing of such parts provided various metal-plastic composite parts having complicated hollow structures with specific topological relationships with the resolution of 40 µm. Using this technique, 3D devices that cannot be manufactured by traditional methods are possible, and metal patterns can be produced inside plastic parts as a means of further miniaturizing electronics. The proposed method can also generate metal coatings exhibiting improved adhesion of metal to substrate. Finally, several sensors composed of different functional materials and specific metal patterns were designed and fabricated. The present results demonstrate the viability of the proposed method and suggest potential applications in the fields of 3D electronics, wearable devices, and sensors.

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Liquid crystal elastomers (LCE) are appealing candidates among active materials for 4D printing, due to their reversible, programmable and rapid actuation capabilities. Recent progress has been made on direct ink writing (DIW) or Digital Light Processing (DLP) to print LCEs with certain actuation. However, it remains a challenge to achieve complicated structures, such as spatial lattices with large actuation, due to the limitation of printing LCEs on the build platform or the previous layer. Herein, a novel method to 4D print freestanding LCEs on-the-fly by using laser-assisted DIW with an actuation strain up to -40% is proposed. This process is further hybridized with the DLP method for optional structural or removable supports to create active 3D architectures in a one-step additive process. Various objects, including hybrid active lattices, active tensegrity, an actuator with tunable stability, and 3D spatial LCE lattices, can be additively fabricated. The combination of DIW-printed functionally freestanding LCEs with the DLP-printed supporting structures thus provides new design freedom and fabrication capability for applications including soft robotics, smart structures, active metamaterials, and smart wearable devices.

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Mechanical metamaterials pave a way for designing and optimizing microstructure topology to achieve counterintuitive deformation including negative Poisson's ratio (NPR) and negative thermal expansion (NTE). Previous studies were always limited to single anomalous mechanical or thermal deformation, but current applications for high-precision mechanical or optical equipment always require their combination and customized and anisotropic deformation parameters. This work develops programmable two-dimensional (2D) mechanical metamaterials based on chiral and antichiral structures constructed with curved bimaterial strips to produce tailorable NPR and arbitrary thermal deformation. The coefficient of thermal expansion of the mechanical metamaterials is tunable on a large scale across negative, near-zero, and positive values depending on the bimaterial configurations and geometrical parameters of curved strips, while the value of NPR is mainly determined by the radian. Furthermore, it is programmable by coding the unit cells to exhibit customized and anisotropic thermal deformation combining homogeneous, gradient, and shear modes. The proposed mechanical metamaterials are fabricated by multimaterial three-dimensional (3D) printing, and the unusual deformation modes are verified experimentally, which is well in agreement with the results of finite element analysis. This work demonstrates a feasible approach to achieving customized mechanical and thermal deformation through easy block building for specific engineering applications including eliminating thermal stress, shape morphing, and smart actuators.

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This review summarizes the most recent advances from technological and physico-chemical perspectives to improve several remaining issues in polymeric materials' additive manufacturing (AM). Without a doubt, AM is experimenting with significant progress due to technological innovations that are currently advancing. In this context, the state-of-the-art considers both research areas as working separately and contributing to developing the different AM technologies. First, AM techniques' advantages and current limitations are analyzed and discussed. A detailed overview of the efforts made to improve the two most extensively employed techniques, i.e., material extrusion and VAT-photopolymerization, is presented. Aspects such as the part size, the possibility of producing parts in a continuous process, the improvement of the fabrication time, the reduction of the use of supports, and the fabrication of components using more than one material are analyzed. The last part of this review complements these technological advances with a general overview of the innovations made from a material perspective. The use of reinforced polymers, the preparation of adapted high-temperature materials, or even the fabrication of metallic and ceramic parts using polymers as supports are considered. Finally, the use of smart materials that enable the fabrication of shape-changing 3D objects and sustainable materials will also be explored.

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Multimaterial additive manufacturing is an attractive way of producing parts with improved functional properties by combining materials with different properties within a single part. Pure Ti provides a high ductility and an improved corrosion resistance, while the Ti64 alloy has a higher strength. The combination of these alloys within a single part using additive manufacturing can be used to produce advanced multimaterial components. This work explores the multimaterial Laser Powder Bed Fusion (L-PBF) of Ti/Ti64 graded material. The microstructure and mechanical properties of Ti/Ti64-graded samples fabricated by L-PBF with different geometries of the graded zones, as well as different effects of heat treatment and hot isostatic pressing on the microstructure of the bimetallic Ti/Ti64 samples, were investigated. The transition zone microstructure has a distinct character and does not undergo significant changes during heat treatment and hot isostatic pressing. The tensile tests of Ti/Ti64 samples showed that when the Ti64 zones were located along the sample, the ratio of cross-sections has a greater influence on the mechanical properties than their shape and location. The presented results of the investigation of the graded Ti/Ti64 samples allow tailoring properties for the possible applications of multimaterial parts.

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Cephalopods use chromatophores distributed on their soft skin to change skin color and its pattern. Each chromatophore consists of a central sac containing pigment granules and radial muscles surrounding the sac. The contraction of the radial muscle causes the central sac to expand in area, making the color of the pigment more visible. With the chromatophores actuating individually, cephalopods can create extremely complex skin color patterns, which they utilize for exquisite functions including camouflage and communication. Inspired by this mechanism, we present an artificial chromatophore that can modulate its color pattern in response to light. Multimaterial projection microstereolithography is used to integrate three functional components including a photoactive hydrogel composite with polydopamine nanoparticles (PDA-NPs), acrylic acid hydrogel, and poly(ethylene glycol) diacrylate. In order to generate light-driven actuation of the artificial chromatophore, the photothermal effect of the PDA-NPs, light-responsive deformation of the photoactive hydrogel composite, and the produced mechanical stresses are studied. Mechanical properties and interfacial bonding strengths between different materials are also investigated to ensure structural integrity during actuation. We demonstrate pattern modulation of the light-responsive artificial chromatophores (LACs) with the projection of different light patterns. The LAC may suggest a new concept for various engineering applications such as the camouflage interface, biophotonic device, and flexible display.

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Magnetic soft materials (MSMs) have shown potential in soft robotics, actuators, metamaterials, and biomedical devices because they are capable of untethered, fast, and reversible shape reconfigurations as well as controllable dynamic motions under applied magnetic fields. Recently, magnetic shape memory polymers (M-SMPs) that incorporate hard magnetic particles in shape memory polymers demonstrated superior shape manipulation performance by realizing reprogrammable, untethered, fast, and reversible shape transformation and shape locking in one material system. In this work, we develop a multimaterial printing technology for the complex structural integration of MSMs and M-SMPs to explore their enhanced multimodal shape transformation and tunable properties. By cooperative thermal and magnetic actuation, we demonstrate multiple deformation modes with distinct shape configurations, which further enable active metamaterials with tunable physical properties such as sign-change Poisson's ratio. Because of the multiphysics response of the M-MSP/MSM metamaterials, one distinct feature is their capability of shifting between various global mechanical behaviors such as expansion, contraction, shear, and bending. We anticipate that the multimaterial printing technique opens new avenues for the fabrication of multifunctional magnetic materials.

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Natural organisms provide inspirations for various functional structures and surfaces with significant applications in multidisciplinary fields. These biological systems are generally composed of multiscale surface structures with high geometric complexity and a variety of materials, making it challenging to replicate their characteristics in engineering. This study presents a novel multiscale multimaterial 3D printing method, magnetic field-assisted stereolithography (M-SL), for fabricating hierarchical particle-polymer structures with surface features ranging from a few nanometers to millimeters or even centimeters. Taking inspiration from nature, this study describes the design and fabrication of a bioinspired multiscale hierarchical surface structure, which is characterized of microscale cones, nanoscale pores, and surface wrinkles at a few nanometers. To understand the fundamental physics underlying the hierarchical surface structure fabrication in the proposed M-SL process, the complexities among the M-SL process parameters, material parameters, and printed geometries are discussed. The accuracy of the developed printing method is investigated by comparing the printed geometries and digital designs. Effects of the printed hierarchical surface structure on hydrophobicity and cell viability were characterized and discussed. It was found that the highly hierarchical surface structure changed the polymer composite surface from hydrophilic (contact angle: ∼38°) to hydrophobic (∼146°). In addition, the hierarchical surface structure also created a better environment for cell attachment and growth, with 900% more living cells at 72 h after cell seeding, compared with cells on the nonstructured smooth surface. Local and selective cell seeding can also be enabled by the surface structure design. Experimental results validated the effectiveness of the M-SL 3D printing method on fabricating multimaterial functional objects with hierarchically structured surfaces for a wide spectrum of applications.

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3D printing with a high degree of spatial and compositional precision could open new avenues to the design and fabrication of functional composites. By combining the direct ink writing and microfluidics, a multimaterial 3D printing system for fabricating textured composites with liquid inclusions of programmable spatial distribution and compositions is reported here. Phase diagrams for the rational selection of desired printing parameters are determined through a combination of simple theoretical analysis and experimental studies. 1D, 2D, and 3D structures programmed with desired inclusion patterns and compositions are fabricated. Moreover, the versatility of this 3D printing framework in fabricating layered composite beams of tunable thermal property and self-healing materials is demonstrated. The proposed multimaterial microfluidic 3D printing framework could be broadly applicable for structural composites and soft robotic devices.

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Hybrid 3D printing is a new method for producing soft electronics that combines direct ink writing of conductive and dielectric elastomeric materials with automated pick-and-place of surface mount electronic components within an integrated additive manufacturing platform. Using this approach, insulating matrix and conductive electrode inks are directly printed in specific layouts. Passive and active electrical components are then integrated to produce the desired electronic circuitry by using an empty nozzle (in vacuum-on mode) to pick up individual components, place them onto the substrate, and then deposit them (in vacuum-off mode) in the desired location. The components are then interconnected via printed conductive traces to yield soft electronic devices that may find potential application in wearable electronics, soft robotics, and biomedical devices.

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Self-transforming structures are gaining prominence due to their general ability to adopt programmed shapes each tailored for specific functions. Composites that self-fold have so far relied on using the stimuli-responsive mechanisms focusing on reversible shape change. Integrating additional functions within these composites can rapidly enhance their practical applicability; however, this remains a challenging problem. Here, we demonstrate a method for spontaneous folding of three-dimensional (3D)-printed composites with embedded electronics at room temperature. The composite is printed using a multimaterial 3D-printing process with no external processing steps. Upon peeling from the print platform, the composite self-shapes itself using the residual forces resulting from polymer swelling during the layer-by-layer fabrication process. As a specific example, electrochromic elements are printed within the composite and can be electrically controlled through its folded legs. Our shape-transformation scheme provides a route to transform planar electronics into nonplanar geometries containing the overhangs. Integrating electronics within complex 3D shapes can enable new applications in sensing and robotics.