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In this study, a sugarcane bagasse biochar/nano-iron oxide composite was prepared via a one-pot pyrolysis method by using the sugarcane bagasse-based solid waste and microwave as the raw material and energy source, respectively. The developed composite was characterized by BET, XRD, FT-IR and TEM and was applied for the removal of Cr (VI) from water. The composite was observed to be mainly composed of amorphous carbon, Fe3O4 and Fe2O3. The iron oxides were uniformly embedded on the surface of the carbon layer by van der Waals force. The sugarcane bagasse-based biochar/nano-iron oxide composite material exhibited an optimal Cr (VI) adsorption capacity of 55 mg/g under the experimental conditions specified in this study. The Cr (VI) adsorption mechanism of the Fe2O3/Fe3O4/WBC composite was explained through FTIR, XPS, charge transfer analyses, and density functional theory calculations (DFT). The deposition of Cr (VI) on the surface of the composite was attributed to electrostatic interaction, redox reactions and complexation between the Fe2O3/Fe3O4/WBC composite and Cr (VI) contained in the solution.