Magnetically separable millimeter-sized chitosan beads containing nanosized gamma-Fe2O3 were prepared for Cr(VI) removal. The magnetism of the beads arises from the gamma-Fe2O3 nanoparticles, by which the sorbent can be easily recovered by the application of an external magnetic field. Various factors influencing the sorption behavior such as pH, temperature, contact time, initial concentration of Cr(VI), and coexisting anions were systematically studied. The time-dependent Cr(VI) sorption data were well described by pseudo-second-order kinetic model. The best interpretation for the equilibrium data was the Freundlich isotherm, and the maximum sorption capacity achieved was 106.5 mg/g at an initial concentration of 200 ppm and pH 5. Thermodynamic parameters of the sorption process were also calculated, which revealed that the sorption of Cr(VI) onto gamma-Fe2O3 chitosan beads was spontaneous and exothermic. The sorbed Cr(VI) can be effectively removed from the sorbent with 0.1 M NaOH. The regeneration of the sorbents was affirmed in six sequential cycles of sorption-desorption experiments, without significant loss in sorption capacity. Furthermore, Cr(VI) loaded sorbent was investigated by means of FTIR and XPS analysis to discuss the uptake mechanism. The uptake mechanism including electrostatic interaction, chelation, and precipitation were found to be involved in the complex sorption of Cr(VI) on the sorbent.