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• The synthesis strategies of ZIFs are briefly introduced and summarized. • Batch experiment, spectral analysis and DFT are used to explore mechanisms. • The mechanisms mainly ascribe to coordination and electrostatic interaction. • Large SSA and sufficient functional groups endow ZIFs excellent performance. • Multi-factor influences demonstrate the practical application potential of ZIFs. With the rapid economic globalization and energy development, heavy metal ions/radionuclides are inevitably discharged into aqueous system and cause pollution, which seriously endanger human health and environmental sustainability. In recent years, zeolitic imidazolate frameworks (ZIFs) with huge specific surface area, excellent pore structure and abundant surface functional groups show great potential in the elimination of heavy metal ions/radionuclides. This review systematically summarizes the research progress of ZIFs and ZIF-based materials for capturing heavy metal ions/radionuclides. Firstly, the preparation and modification of ZIF-based materials are briefly introduced. Then, the removal behaviors and possible interaction mechanisms between ZIF-based materials and pollutants are explored through macro-batch experiments, micro-spectroscopy analyses and theoretical calculations. In addition, the partition coefficient as evaluation indicator was employed to objectively compare the removal performance of ZIFs and other commonly used traditional adsorbents for heavy metal ions/radionuclides. Finally, the challenges and prospects of ZIF materials in environmental governance are briefly discussed so as to provide references for future research and practical applications. [ABSTRACT FROM AUTHOR]