To enhance the adsorption performance of chitosan for rare earth ions, two novel magnetic chitosan-based adsorbents were prepared by using chitosan-coated magnetic silica nanoparticles modified with amine-thiourea and aniline. The structure of copolymers was analyzed using characterization methods such as X-ray diffraction, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and thermogravimetric analysis, confirming the successful synthesis of modified magnetic chitosan nanocomposites. The investigation explored the influence of pH, contact time, dosage, initial concentration, and temperature on the adsorption performance. Comparative studies revealed a significantly enhanced adsorption performance after modification. The chitosan-coated magnetic silica nanoparticles modified with aniline (PAN-CS/Fe3O4@SiO2) reached adsorption saturation in about 120 min with a capacity of 136 mg/g, while the chitosan-coated magnetic silica nanoparticles modified with amine-thiourea (TSC-CS/Fe3O4@SiO2) exhibited a higher adsorption capacity of 156 mg/g for Ce(III). Both materials demonstrated strong agreement with the Langmuir isotherm model and pseudo-second-order kinetics. Thermodynamic analysis indicated that Ce(III) adsorption is both spontaneous and endothermic. Examination of the adsorption mechanisms suggested that the effective adsorption of Ce(III) is due to the strong synergistic effects of chelation and electrostatic interactions involving amino, carboxyl, and hydroxyl groups. This study demonstrates that chitosan modified with amine-thiourea and aniline is an effective approach to significantly enhance the rare earth ion adsorption by chitosan.