Nanoscale zero-valent iron (NZVI) and NZVI supported onto montmorillonite (NZVI-Mt) were synthetized and used in this study to remove Se^VI and As^V from water in mono- and binary-adsorbate systems. The adsorption kinetics and isotherm data for Se^VI and As^V were adequately described by the pseudo-second-order (PSO) (r²>0.94) and Freundlich (r²>0.93) equations. Results from scanning electron microscopy showed that the dimension of the NZVI immobilized on the Mt was smaller than pure NZVI. Using 0.05 g of adsorbent and an initial 200 mg L−1 As^V and Se^VI concentration, the maximum adsorption capacity (q_max) and partition coefficient (PC) for As^V on NZVI-Mt in monocomponent system were 54.75 mg g^-1 and 0.065 mg g^-1·μM^-1, which dropped respectively to 49.91 mg g^-1 and 0.055 mg g^-1·μM^-1 under competitive system. For Se^VI adsorption on NZVI-Mt in monocomponent system, q_max and PC were 28.63 mg g^-1 and 0.024 mg g^-1·μM^-1, respectively. Values of q_max and PC were higher for NZVI-Mt than NZVI and montmorillonite, indicating that the nanocomposite contained greater adsorption sites for removing both oxyanions, but with a marked preference for As^V. Future research should evaluate the effect of different operational variables on the removal efficiency of both oxyanions by NZVI-Mt.