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Metal–organic frameworks (MOFs) with Lewis acid catalytic sites, such as zirconium‐based MOFs (Zr‐MOFs), comprise a growing class of phosphatase‐like nanozymes that can degrade toxic organophosphate pesticides and nerve agents. Rationally engineering and shaping MOFs from as‐synthesized powders into hierarchically porous monoliths is essential for their use in emerging applications, such as filters...