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Highly porous zeolitic imidazolate frameworks (ZIFs), with disparate metal ions (ZIF-8 and ZIF-67), disparate organic ligands (ZIF-9 and ZIF-67), single or double central metal atoms (ZIF-8, Zn/Co-ZIF and ZIF-67) were prepared and used in the elimination of typical radionuclide U(VI). The detailed interaction mechanisms were studied by batch experiments, spectral analyses and DFT calculation. Langmuir isotherms model revealed a decreasing tendency to remove U(VI): ZIF-8 (540.4 mg/g) > Zn/Co-ZIF (527.5 mg/g) > ZIF-9 (448.6 mg/g) > ZIF-67 (368.2 mg/g). Based on the effects of pH and foreign ions, FTIR and XPS spectra analyses, the possible interaction mechanisms of U(VI) onto ZIFs were surface complexation and electrostatic interaction. Among them, ZIF-8 with Zn metal center and 2-methylimidazolate organic ligand had the best elimination capacity for U(VI) because of its large surface area, active metal ion and abundant nitrogen-containing groups (e.g., C–N, Zn–N and C N). Specially, the adsorption energy of ZIF-8-Zn2-UO 2 2+ structure was −2.299 eV obtained by DFT calculation, illustrating that U(VI) and N atoms were formed the most stable bidentate coordination compounds. This paper highlights the effects of the hydroxylated metals, the functional groups of the imidazole ring on the elimination of U(VI), which can provide constructive suggestions for further adsorbent materials amelioration. Image 1 • ZIF-8, ZIF-9, ZIF-67 and Zn/Co-ZIF were fabricated by stirring at room temperature. • Excellent structural performances endowed four ZIFs outstanding sorption capacity. • The differences in adsorption mechanism of four ZIFs were investigated in detail. • The N atoms of ZIF-8 formed bidentate coordination compounds with U(VI). [ABSTRACT FROM AUTHOR]