U and Th have attracted a great deal of attention due to their potential application as nuclear fuel materials. For the first time, we report here the synthesis and sorption of diglycolamic acid monoamidefunctionalized metal organic framework (MOF), UiO-66-NH-CODGAMA (MOFDGAMA), as a robust sorbent for the efficient removal of UO 2 2+ and Th 4+ . Introduction of the DGAMA group remarkably enhances the sorption capacity for both UO 2 2+ (193 mg g −1 ) and Th 4+ (227 mg g −1 ) compared to pristine UiO-66-NH 2 . MOFDGAMA was found to exhibit high radiolytic stability and good recyclability over multiple cycles for the efficient extraction of hexavalent uranium (UO 2 2+ ) and tetravalent thorium (Th 4+ ) from aqueous acidic streams. The findings of this work demonstrate the potential application of the materials to remove radionuclides from nuclear effluents.