AbstractIn this study, the hierarchical mesoporous carbon (HMC) was synthesized by the hydrothermal method. The batch adsorption experiments showed that HMC exhibited the ultrafast equilibrium fate (80 % U(VI) capture efficiency within 5 min), high UO22+ capture capacity (210 mg/g, pH = 4.5) and well recyclability. The investigations of XPS techniques indicated the oxygen-containing functional groups were responsible for high efficient UO22+ adsorption. The pH-dependent adsorption was simulated by three surface complexation modellings, revealing that UO22+ adsorption on HMC was excellently fitted by triple layer model using two inner-sphere complexes (i. e. SOUO2+ and SOUO2(CO3)35− species) compared to constant capacitance model and diffuse layer model. These findings are crucial for expanding actual applications of HMC towards the removal of radionuclides under environmental cleanup.