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Natural PCET enzyme catalysis generally requires tripartite preorganization of proton relay, substrate\u2010bound active center, and redox mediator, making the processes efficient and precluding side reactions. Inspired by this, a heterogeneous photocatalytic PCET system was established to achieve higher PCET driving forces by modifying proton relays into anthraquinone\u2010based anionic coordination polymers. The proximally separated proton relays and photoredox\u2010mediating anthraquinone moiety allowed pre\u2010assembly of inert substrate between them, merging proton and electron into unsaturated bonds by photoreductive PCET, which enhanced reaction kinetics compared with the counter catalyst without proton relay. This photocatalytic PCET method was applied to a broad\u2010scoped reduction of aryl ketones, unsaturated carbonyls, and aromatic compounds. 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