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This review traces the development of MOF\u2010based phosphatase catalysts from the fundamental principles of biological phosphate ester hydrolysis to their practical application in degrading organophosphorus pollutants and chemical warfare agents. The mechanistic challenges of activating the phosphorus center are discussed, with particular attention to the roles of metal ion Lewis acidity, coordination environment, and active\u2010site architecture in governing catalytic activity. The structural advantages of MOFs are examined in the context of phosphate hydrolysis catalysis. Major MOF families and key structure\u2013activity relationships, including node connectivity, defect engineering, and linker functionality, are discussed to provide mechanistic insight. The review further covers MOF phosphatase applications in detoxifying organophosphate pesticides and nerve agents, highlighting advances in solution\u2010phase catalysis and solid\u2010state decontamination. 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