Chitosan modified with ethylenediamine molecules has been evaluated as an effective adsorbent for Cr(VI) ions from aqueous system. The removal of Cr(VI) by adsorption was investigated at different pH conditions using UV-Vis spectrophotometry. The adsorption data were interpreted based on the Langmuir, Freundlich, and Temkin isotherm models. The isotherm constants were evaluated. The maximum adsorption capacity obtained from Langmuir model is 90.3 mg g(-1) at 323 K and pH-3.0. The adsorption process was evaluated using the pseudo first-order, pseudo second-order, and intra-particle diffusion models and is observed to follow second order kinetics. The thermodynamic parameters of adsorption were evaluated. The result indicated the adsorption process to be spontaneous and endothermic. The sorbent was successfully regenerated using 0.5N NaOH and its reusability has been evaluated.