In this study, organobentonites were prepared by modification of bentonite with various cationic surfactants, and were used to remove As (V) and As (III) from aqueous solution. The results showed that the adsorption capacities of bentonite modified with octadecyl benzyl dimethyl ammonium (SMB3) were 0.288 mg/g for As (V) and 0.102 mg/g for As (III), which were much higher compared to 0.043 and 0.036 mg/g of un-modified bentonite (UB). The adsorption kinetics were fitted well with the pseudosecond-order model with rate constants of 46.7×10−3g/mg h for As (V) and 3.1×10−3g/mg h for As (III), respectively. The maximum adsorption capacity of As (V) derived from the Langmuir equation reached as high as 1.48 mg/g, while the maximum adsorption capacity of As (III) was 0.82mg/g. The adsorption of As (V) and As (III) was strongly dependent on solution pH. Addition of anions did not impact on As (III) adsorption, while they clearly suppressed adsorption of As (V). In addition, this study also showed that desorbed rates were 74.61% for As (V) and 30.32% for As (III), respectively, after regeneration of SMB3 in 0.1M HCl solution. Furthermore, in order to interpret the proposed absorption mechanism, both SMB3 andUBwere extensively characterized using scanning electron microscopy (SEM), X-ray diffraction (XRD) and Fourier transform infrared (FTIR) analyses.