The development of nanomaterials incorporating organic components holds significant importance in addressing the efficient removal of metal ions through adsorption. Hence, in this study, a novel MnFe2O4/chitosan/Schiff base nanocomposite was successfully synthesized by crosslinking MnFe2O4 nanoparticles with functionalized chitosan using a novel Schiff base. The Schiff base was created through the condensation reaction between 2-aminophenol and terephthalaldehyde. Comprehensive characterization of the synthesized nanocomposite was performed through FT-IR, XRD, SEM, and VSM analyses, revealing a less crystalline arrangement compared to pure chitosan, a rough and non-uniform surface morphology, and a reduced magnetization value of 30 emu/g. Furthermore, the synthesized MnFe2O4/chitosan/Schiff base nanocomposite was working as an adsorbent for the effective disposal of Zn(II) ions from aqueous solutions. The synthesized nanocomposite exhibited a maximum sorption capacity of 289.86 mg/g for Zn(II) ions. Additionally, the results indicated that the removal of Zn(II) ions by the synthesized nanocomposite was a spontaneous, chemical, and endothermic process, aligning well with the Langmuir isotherm as well as the pseudo-second-order model. Furthermore, at pH 7.5, with a contact duration of 100 min and a temperature of 328 K, the fabricated nanocomposite reached its maximum sorption capacity for Zn(II) ions. The results of this study demonstrate the effectiveness of the newly synthesized MnFe2O4/chitosan/Schiff base nanocomposite in removing Zn(II) ions from aqueous media. The novel synthesis approach and the high adsorption capacity of 289.86 mg/g underscore the potential of this composite for practical applications in industrial wastewater treatment. The dual removal mechanism involving electrostatic attraction and complexation processes further enhances its utility, making it a valuable contribution to the field of environmental remediation.