Two cationic polymer-epicholorohydrin dimethylamine (EPI-DMA) and poly dimethyldlammonium (PDMDAAC) as the intercalary reagents were used to prepare a series of bentonites (EPI-DMA/Bt and PDMDAAC/Bt) modified by the cationic polymers, respectively. The adsorption of Cr(VI) on cationic polymer/bentonite and major influencing factors were studied. The results show that the sorption capacity of Cr (VI) is increased more than five times compared with the original one. The load of cationic polymers in bentonites, the dosing quantity of EPI-DMA/Bt and PDMDAAC/Bt, the solution pH, temperature (T), time of reaction (t) affect the adsorption. When T = 20 degrees C, pH = 4.0, t = 120 min, EPI-DMA/Bt (the load of cationic polymer is 99.6 mg/g) and PDMDAAC/Bt (the load of cationic polymer is 55.1 mg/g) adsorb 0.71 mg/g and 0.56 mg/g Cr(VI), respectively. The adsorption kinetics are fitted well by pseudo second-order equation. The adsorption isotherms of cationic polymer/bentonites to Cr( VI) are fitted well by the Langmuir equation.