Nano zero-valent manganese (nZVMn) is theoretically expected to exhibit high reducibility and adsorption ca-pacity, yet its feasibility, performance, and mechanism for reducing and adsorbing hexavalent uranium (U(VI)) from wastewater remain unclear. In this study, nZVMn was prepared via borohydride reduction, and its be-haviors about reduction and adsorption of U(VI), as well as the underlying mechanism, were investigated. Results indicated that nZVMn exhibited a maximum U(VI) adsorption capacity of 625.3 mg/g at a pH of 6 and an adsorbent dosage of 1 g/L, and the co-existing ions (K+, Na+, Mg2+, Cd2+, Pb2+, Tl+, Cl-) at studied range had little interference on U(VI) adsorption. Furthermore, nZVMn effectively removed U(VI) from rare-earth ore leachate at a dosage of 1.5 g/L, resulting in a U(VI) concentration of lower than 0.017 mg/L in the effluent. Comparative tests demonstrated the superiority of nZVMn over other manganese oxides (Mn2O3 and Mn3O4). Characterization analyses, including X-ray diffraction and depth profiling X-ray photoelectron spectroscopy, combined with density functional theory calculation revealed that the reaction mechanism of U(VI) using nZVMn involved reduction, surface complexation, hydrolysis precipitation, and electrostatic attraction. This study provides a new alternative for efficient removal of U(VI) from wastewater and improves the understanding of the interaction between nZVMn and U(VI).