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Inspired by biology, in which a bimetallic hydroxide‐bridged zinc(II)‐containing enzyme is utilized to catalytically hydrolyze phosphate ester bonds, the utility of a zirconium(IV)‐cluster‐containing metal–organic framework as a catalyst for the methanolysis and hydrolysis of phosphate‐based nerve agent simulants was examined. The combination of the strong Lewis‐acidic Zr^IV and bridging hydroxide anions led to ultrafast half‐lives for these solvolysis reactions. This is especially remarkable considering that the actual catalyst loading was a mere 0.045 % as a result of the surface‐only catalysis observed.