Super-paramagnetic iron oxide nanoparticles (SPIONs)/gelatin (gel)/polyvinyl alcohol (PVA) nanoparticles were designed and synthesized by the co-precipitation method and further modified with gel and PVA. These nanoparticles were used for the removal of Cu(II) and Zn(II) from aqueous solutions. The adsorbents were rich in different functional groups for chemisorption and showed effective adsorption properties. The adsorption of Cu(II) and Zn(II) on the SPIONs/gel and SPIONs/gel/PVA materials were investigated with respect to pH, adsorption kinetics, and adsorption isotherms. The adsorption data was fitted to the Langmuir, Freundlich, and Sips models at the optimum pH 5.2 (±0.2) over 60 min; SPIONs/gel showed maximum adsorption capacities of 47.594 mg/g and 40.559 mg/g for Cu(II) and Zn(II); SPIONs/gel/PVA showed those of 56.051 mg/g and 40.865 mg/g, respectively. The experimental data fitted the pseudo-second-order model, indicating that the process followed chemical monolayer adsorption. In addition, the SPIONs/gel/PVA showed better stability and Cu(II) adsorption efficiency than SPIONs/gel.