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Both environment and human beings were menaced by the widespread application of radioactive uranium, high-performance and effective elimination of uranium from wastewater is of important meaning for development of environmental sustainability in the future. In this study, the water-stable MOF material and the highly crystalline COF were compounded by a mild hydrothermal strategy, which achieved efficient removal of U(VI) through the synergistic effect. The composites showed the characteristics of both COFs and MOFs, which will possess higher stability, larger surface area and faster adsorption efficiency that cannot be carried out by a single component. Batch experiments and characterizations (SEM, TEM, XRD, FT-IR, BET, XPS, etc.) indicated that UiO-66-NH 2 @LZU1 had more stable and multi-layer pore structure and rich active functional groups. The Langmuir model and the pseudo-second-order kinetics fitting was more suitable for the U(VI) elimination process. The greatest uranium adsorbing capacity of UiO-66-NH 2 @LZU1 (180.4 mg g−1) was observed to exceed the UiO-66-NH 2 (108.8 mg g−1) and COF-LZU1 (65.8 mg g−1), which reached the excellent hybrid effects. Furthermore, FT-IR and XPS analyses confirmed that the most nitrogen-containing group from COF-LZU1 and oxygen-containing group of UiO-66-NH 2 could be combined with U(VI). In addition, electrostatic interaction was also a mechanism during the removal process. This work displayed that UiO-66-NH 2 @LZU1 was a prospective hybrid material for radioactive waste remediation. The compound method and application mentioned in this work had provided a theoretical basis for designing and developing multi-functional composite adsorbents, which contributed to the development of new materials for radioactive wastewater treatment technologies. [Display omitted] • UiO-66-NH 2 @LZU1 composite material was obtained by solvothermal method. • Highly efficient uranium adsorbent, adsorption capacity reached 163.1 mg g−1. • Abundant nitrogen/oxygen functional groups promote uranium removal. • Main removal mechanism included electrostatic interaction and surface complexation. [ABSTRACT FROM AUTHOR]