In this work, montmorillonite (Mt) was modified by environmentally friendly arginine (Arg) and lysine (Lys) amino acids with di-cationic groups for arsenic removal from contaminated water. The modified Mts were characterized by X-ray diffraction, Fourier transform infrared spectroscopy, zeta potential and thermal analysis. The adsorption of As(V) onto modified Mts as a function of initial As(V) concentration, contact time and solution pH was investigated. The removal efficiency was increased with increasing the As(V) concentration and contact time; however, it was decreased with increasing solution pH. The maximum As(V) adsorption capacities of Mt-Arg and Mt-Lys were 11.5 and 11 mg/g, respectively, which were five times larger than pristine Mt. The high adsorption capacity makes them promising candidates for arsenic removal from contaminated water. The regeneration studies were carried out up to 10 cycles for both modified Mts. The obtained results confirmed that the modified adsorbents could also be effectively used for As(V) removal from water for multiple adsorption – desorption cycles.