Covalent organic frameworks (COFs), assembling through covalent bonds, are a rising class of porous materials. Nowadays, various COFs are widely applied in organic pollutants decontamination due to the outstanding capabilities of large surface area, multiple functional groups, porous structure, excellent absorptivity, flexible design and so on. This review concentrates on the applications of COFs in different decontamination technologies such as solid-phase extraction, membrane filtration and sieving, adsorption, and catalysis reaction. The factors influencing water chemistry, such as pH, temperature, salt concentration and natural organic matter, are summarized in terms of their impact on decontamination performance and the extraction mechanisms for the diverse analytes. The interaction mechanisms between COFs and organic pollutants were hydrogen bonding, π-π stacking, hydrophilic, hydrophobic, and electrostatic interactions. Furthermore, a perspective on current obstacles and upcoming developments of COFs for organic pollutant removal has been provided. Due to their adaptable and versatile design as well as elaborate and diverse functionalization, COFs possess significant possibility in ameliorating environmental pollution.