Water pollution by hexavalent chromium (Cr(VI)) is widespread and problematic. As a result, more research into economic Cr(VI) removal is needed. In this study, we created and employed an adsorption–reduction mechanism to remove Cr(VI). Magnetically reduced graphene oxide bentonite (MrGO-BT) is acid resistant and can undergo magnetic separation. The hydroxyl group of chitosan (CS) condensed with the functional groups on the surface of bentonite (BT), and the MrGO-BT sandwich has been fabricated and constructed from an Fe3O4 core layer sandwiched by reduced graphene oxide (rGO) and a BT shell, with CS acting as a crosslinker. Cr(VI) elimination by MrGO-BT was exothermic and spontaneous according to thermodynamic analyses. The adsorption kinetics and adsorption isotherms were characterized by the pseudo-second order kinetic theory and the Langmuir model, respectively. Regarding the elimination of Cr(VI), the greatest adsorption ability for Cr(VI) elimination achieved was 91.5 mg g–1. Fourier-transform infrared spectroscopy and X-ray photoelectron spectroscopy suggested that Cr(VI) was reduced by C–O–H on MrGO-BT to produce Cr(III) and H–C=O, and that Cr(III) chelated with amino groups or exchanged with BT after intercalation. In addition, the introduction of Cu2+ increased the positive charge of MrGO-BT and amplified the electrostatic interaction between Cr2O72− and HCrO4–, which is what caused Cr(VI) to be eliminated. Cu2+ and reduced Cr(III) combined with -NH2 on the surface of MrGO-BT to form -NH-Cr(III) or -NH-Cu2+, and Cr(VI) elimination via chelation and ion exchange was confirmed. MrGO-BT is shown to be an adsorbent with high acid resistance and good magnetic responsiveness and stability.