Cerium vanadate/modified bentonite (CeVO4/mbt) nanocomposite with different composition percentages was synthesized through a simple one-step hydrothermal method at 180 ℃, and then its photocatalytic activity was evaluated by decolorizing methylene blue (MB) in an aqueous solution under light exposure. In order to increase the surface area as an important parameter in photocatalytic processes, bentonite was modified by ball mill method. The structural and optical properties of the synthesized composites were determined by XRD, FT-IR, DRS, FESEM, EDS, and BET measurements. XRD and EDS results confirmed the successful synthesis of pure CeVO4. FESEM images and EDS mapping showed a proper distribution of rice-like CeVO4 nanoparticles on bentonite. The removal efficiency of MB with only 0.1 g of CeVO4/mbt nanocomposite in 15 min was about 99%, which is significant compared to neat bentonite and pure CeVO4 with efficiency of 30% and 57%. The mentioned nanocomposite followed the first-order kinetics, had a reaction rate constant equal to 0.1483 min–1, and showed acceptable stability in five consecutive cycles.