Biosorption is a technique widely used in the remediation of contaminated effluents, and its main advantages are its easy applicability, high efficiency rate, versatility, and its economic viability. Associated with nanotechnology, this work proposes the use of nanocomposites of sugarcane bagasse (SB) and ferromagnetic nanoparticles (Fe3O4) in the removal of metallic ions present in contaminated water. SB is a promising adsorbent material since it is an abundant agricultural residue, easily accessed. By using the coprecipitation method, two nanocomposites were obtained from in natura (SB-NP) or acid-treated (MSB-NP) sugarcane bagasse. These materials were synthetized by impregnation of Fe3O4 to gain paramagnetic properties and to facilitate the removal of the contaminant-containing adsorbent. The characterization of the nanocomposites was performed using pHPCZ, FTIR, XRD, and SEM/EDS techniques, to evaluate the synthesis efficiency and investigate the morphology of the materials. The efficiency of magnetite impregnation on the SB was assessed by SEM/EDS and XRD, while the main functional groups (carbonyl, carboxyl, hydroxyl, amine, amide, and nitrate) responsible for adsorption were found by FTIR. In the surface charge characterization by pHPCZ sorption of dyes, it was found that negative charges are predominant. The pHPCZ for SB-NP and MSB-NP was 5.95 and 5.59, respectively, and the chosen Cu(II) adsorption pH was 6.2 ± 0.1. The adsorption equilibrium was reached between 10 and 60 min of contact time. The maximum experimental sorption capacity (SCexp) was 2.53 ± 0.09 (SB-NP) and 2.61 ± 0.01 mg/g (MSB-NP). The isotherm models applied to the experimental data were Langmuir, Freundlich, Sips, Temkin, and Dubinin-Radushkevich, and Temkin best described the adsorption phenomena for Cu(II) by SB-NP (r2 = 0.9976 and χ2 = 3.965) and MSB-NP (r2 = 0.9990 and χ2 = 1.816). Reuse cycles of the nanocomposites were also performed employing ten cycles of sorption using 50 mg/L Cu(II) solutions, after which the materials showed SCexp = 7.47 ± 0.04 mg/g (SB-NP) and 7.82 ± 0.04 mg/g (MSB-NP). Therefore, the investigated materials exhibited promising results to be used as biosorbents in the remediation of effluents contaminated with toxic metal ions, such as copper.