Bentonite is a natural clay that presents characteristics such as good capacity to exchange cations, large specific surface area, large porosity, and possibility to undergo intercalation and/or functionalization. This work reports on bentonite functionalization with organomodified alkoxides. Functionalization afforded hybrid materials displaying desirable properties for adsorption of chromium trivalent ions. Infrared absorption spectroscopy, X-ray powder diffraction, thermal analysis, specific surface area analysis, and adsorption experiments with methylene blue helped to characterize the materials and evaluate their cationic exchange capability. These techniques evidenced functionalization of the Brazilian bentonite. Kinetic and equilibrium experiments on the adsorption of chromium trivalent ions aided determination of the equilibrium time of kinetic adsorption isotherms and revealed whether the functionalized matrices adsorbed chromium trivalent ions. Chromium displayed S1 type adsorption isotherms, which confirmed that adsorption capacity originated from cooperative forces between the adsorbate and the hybrid adsorbents.