The recovery of strategic metals such as rare earth elements (REEs) requires the development of new sorbents with high sorption capacities and selectivity. The bi-functionality of sorbents showed a remarkable capacity for the enhancement of binding properties. This work compares the sorption properties of magnetic chitosan (MC, prepared by dispersion of hydrothermally precipitated magnetite microparticles (synthesized through Fe(II)/Fe(III) precursors) into chitosan solution and crosslinking with glutaraldehyde) with those of the urea derivative (MC-UR) and its sulfonated derivative (MC-UR/S) for cerium (as an example of REEs). The sorbents were characterized by FTIR, TGA, elemental analysis, SEM-EDX, TEM, VSM, and titration. In a second step, the effect of pH (optimum at pH 5), the uptake kinetics (fitted by the pseudo-first-order rate equation), the sorption isotherms (modeled by the Langmuir equation) are investigated. The successive modifications of magnetic chitosan increases the maximum sorption capacity from 0.28 to 0.845 and 1.25 mmol Ce g−1 (MC, MC-UR, and MC-UR/S, respectively). The bi-functionalization strongly increases the selectivity of the sorbent for Ce(III) through multi-component equimolar solutions (especially at pH 4). The functionalization notably increases the stability at recycling (for at least 5 cycles), using 0.2 M HCl for the complete desorption of cerium from the loaded sorbent. The bi-functionalized sorbent was successfully tested for the recovery of cerium from pre-treated acidic leachates, recovered from low-grade cerium-bearing Egyptian ore.