Nanomaterial-based wound dressings have been extensively studied for the treatment of both minor and life-threatening tissue injuries. These wound dressings must possess several crucial characteristics, such as tissue compatibility, non-toxicity, appropriate biodegradability to facilitate wound healing, effective antibacterial activity to prevent infection, and adequate physical and mechanical strength to withstand repetitive dynamic forces that could potentially disrupt the healing process. Nevertheless, the development of nanostructured wound dressings that incorporate various functional micro- and nanomaterials in distinct architectures, each serving specific purposes, presents significant challenges. In this study, we successfully developed a novel multifunctional wound dressing based on poly(lactic acid) (PLA) fibrous membranes produced by solution-blow spinning (SBS) and electrospinning. The PLA-based membranes underwent surface modifications aimed at tailoring their properties for utilization as effective wound dressing platforms. Initially, beta-chitin whiskers were deposited onto the membrane surface through filtration, imparting hydrophilic character. Afterward, silver nanoparticles (AgNPs) were incorporated onto the beta-chitin layer using a spray deposition method, resulting in platforms with antimicrobial properties against both Staphylococcus aureus and Escherichia coli. Cytotoxicity studies demonstrated the biocompatibility of the membranes with the neonatal human dermal fibroblast (HDFn) cell line. Moreover, bilayer membranes exhibited a high surface area and porosity (> 80%), remarkable stability in aqueous media, and favorable mechanical properties, making them promising candidates for application as multifunctional wound dressings.