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Synergistic catalytic effects and metal node modulation are pivotal to the performance of multifunctional catalysts.We present a versatile strategy for constructing bimetallic M1M2 cluster catalysts (polyoxometalates (POMs)/Zr‐based metal‐organic frameworks (Zr‐MOF); M1 = Zr; M2 = W, V, Mo) by a microwave‐assisted in‐situ precoordination‐postmodification approach, which consisted of the grafting of...