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While the microenvironment around catalytic sites is recognized to be crucial in thermocatalysis, its roles in photocatalysis remain subtle. In this work, a series of sandwich‐structured metal–organic framework (MOF) composites, UiO‐66‐NH2@Pt@UiO‐66‐X (X means functional groups), is rationally constructed for visible‐light photocatalytic H2 production. By varying the ─X groups of the UiO‐66‐X shell,...