Robust and simple composite films for the removal of methyl orange (MO) and Cr(VI) have been prepared by combining chitosan, saponin, and bentonite at a specific ratio. There are several composite films (chitosan-saponin-bentonite (CSB)) prepared; among them, the composite films CSB2:3 and CSB1:1 have the highest removal efficiency toward MO and Cr(VI) where the maximum removal is 70.4% (pH 4.80) and 92.3% (pH 5.30), respectively. It was found that different types of adsorbate have different thermodynamic properties of the adsorption process; the adsorption of MO onto CSB2:3, chitosan, and acid-activated bentonite (AAB) proceeded endothermically, while the adsorption of Cr(VI) onto CSB1:1, chitosan, and AAB proceeded exothermically. The parameters of the adsorption were modeled by using isotherm and kinetic equations. The models of Langmuir, Freundlich, Redlich-Peterson, Sips, and Toth were used for fitting the adsorption isotherm data at a temperature of 30, 45, and 60 °C; all of the isotherm models could represent the data well. The result indicates that CSB2:3 has the highest adsorption capacity toward MO with qm of 360.90 mg g-1 at 60 °C; meanwhile, CSB1:1 has the highest adsorption capacity toward Cr(VI) with qm 641.99 mg g-1 at 30 °C. The pseudo-second-order model could represent the adsorption kinetics data better than the pseudo-first-order equation. The adsorption mechanism was proposed, and the thermodynamic properties of the adsorption were also studied.