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Environmental pollution is one of the most serious problems facing mankind today, and has attracted widespread attention worldwide. The burgeoning class of crystalline porous organic framework materials, metal-organic frameworks and covalent organic frameworks present promising application potential in areas related to pollution control due to their interesting surface properties. In this review, the literature of the past five years on the adsorptive removal of various hazardous materials, mainly including heavy metal ions, harmful gases, organic dyes, pharmaceutical and personal care products, and radionuclides from the environment by using COFs and MOFs, is summarized. The adsorption mechanisms are also discussed to help understand their adsorption performance and selectivity. Additionally, some insightful suggestions are given to enhance the performance of MOFs and COFs in the adsorptive removal of various hazardous materials.