Efficient removal of U(VT) from mine radioactive wastewater is important for environmental remediation and radiation protection. In this work, a new series of polyamidoxime/polydopamine-decorated graphene oxide (GO/PDA/PAO) composites were obtained by one-pot synthesis and used for the removal of U(VI) from mine radioactive wastewater. The as-synthesized GO/PDA/PAO composites (GO/PDA/PAO-0.2, GO/PDA/PAO-0.5, and GO/PDA/PAO-1) were examined by transmission electron microscopy, Fourier transform infrared (FT-IR), and X-ray photoelectron spectroscopy (XPS). The effects of pH, ionic strength, contact time, initial U(VI) concentration, and temperature on the adsorption behavior of U(VI) by GO/PDA/PAO were investigated. The maximum adsorption capacity of GO/PDA/PAO-0.2 was 502.5 m g/g at pH 6.0 and 298 K. The adsorption kinetics and isotherms can be well illustrated by the pseudo-second-order kinetics model and Langmuir isotherm model. The thermodynamic study indicated that the removal of U(VI) by GO/PDA/PAO-0.2 was an endothermic and spontaneous process. The interactions between GO/PDA/PAO-0.2 and U(VI) were explained based on the FT-IR and XPS analyses. Furthermore, GO/PDA/PAO was applied for U(VI) removal from mine radioactive wastewater. The concentration of U(Vl) in the wastewater can be reduced to 7.28 /mu g/L, which is below the allowable uranium concentration for drinking water stipulated in the standard by the World Health Organization (30 mu g/L).