Carbon-encapsulated Fe/Fe₃C nanoparticles embedded in porous carbon sheets (Fe/Fe₃C@PCS) were fabricated by a one step carbothermic reduction, using natural abundant biomass derivatives. Batch experimental results showed that Fe/Fe₃C@PCS could effectively remove the radionuclide U(VI) from simulated wastewater in the presence of carbonate or calcium under laboratory conditions with reduced cost, improved activity and enhanced kinetics. Compared with activated carbon (AC), Fe/Fe₃C@PCS is more efficient, and can remove U(VI) quantitatively at an initial concentration of up to 140 mg L⁻¹. The major reaction pathway involved the reduction of U(VI) to the insoluble U(IV) species as identified by X-ray photoelectron spectroscopy (XPS) analysis. This study demonstrated the potential application of Fe/Fe₃C@PCS as a low cost and effective remediation strategy for U-contaminated wastewater cleanup.