Magnetic nano-based sorbents have been synthesized for the recovery of two rare earth elements (REE: Nd(III) and Yb(III)). The magnetic nano-based particles are synthesized by a one-pot hydrothermal procedure involving co-precipitation under thermal conditions of Fe(III) and Fe(II) salts in the presence of chitosan. The composite magnetic/chitosan material is crosslinked with epichlorohydrin and modified by grafting alanine and serine amine-acids. These materials are tested for the binding of Nd(III) (light REE) and Yb(III) (heavy REE) through the study of pH effect, sorption isotherms, uptake kinetics, metal desorption and sorbent recycling. Sorption isotherms are well fitted by the Langmuir equation: the maximum sorption capacities range between 9 and 18 mg REE g−1 (at pH 5). The sorption mechanism is endothermic (positive value of ΔH∘) and contributes to increase the randomness of the system (positive value of ΔS∘). The fast uptake kinetics can be described by the pseudo-second order rate equation: the equilibrium is reached within 4 hours of contact. The sub-micron size of sorbent particles strongly reduces the contribution of resistance to intraparticle diffusion in the control of uptake kinetics. Metal desorption using acidified thiourea solutions allows maintaining sorption efficiency for at least four successive cycles with limited loss in sorption capacity.