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Translating this logic to electrosynthesis is attractive from a sustainability perspective because better coupling between proton and electron flow can lower overpotentials, suppress wasteful side reactions, and improve selectivity. Yet, electrochemical MS\u2010PCET remains underexploited, particularly beyond O\u2500H and N\u2500H activation. One of the persistent barriers is molecularity: productive oxidative PCET often requires the simultaneous engagement of three components, a substrate (X\u2013H), an oxidant (Y), and a base (B). Termolecular encounters are entropically disfavored, so practical systems often require molecularity to be engineered down through preorganization. Here, we take a molecularity\u2010based view of electrochemical PCET and classify oxidative PCET into three types based on which pair is preassembled: Type I (X\u2500H\u22efB), Type II (X\u2500H\u22efY), and Type III (Y\u22efB). For each type, reducing molecularity opens a concerted channel, with feasibility determined by the BDFE gap between the donor\/acceptor pair and the target X\u2500H bond. We then discuss representative advances in electrochemical N\u2500H\/O\u2500H activation, M\u2500H generation, and emerging C\u2013H PCET, and conclude with prospects for C\u2500H bond, electrosynthesis, molecularity, PCET, metal hydride interfacial PCET, and asymmetric catalyst design enabled by molecularity engineering.<\/jats:p>","DOI":"10.1002\/chem.202600038","type":"journal-article","created":{"date-parts":[[2026,7,10]],"date-time":"2026-07-10T06:25:09Z","timestamp":1783664709000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Molecularity Control in Electrochemical Multi\u2010Site Proton\u2010Coupled Electron Transfer Reactions"],"prefix":"10.1002","volume":"32","author":[{"given":"Siyu","family":"Chen","sequence":"first","affiliation":[{"name":"Shenzhen Grubbs Institute and Department of Chemistry, Guangming Advanced Research Institute, and Guangdong Provincial Key Laboratory of Catalysis Southern University of Science and Technology  Shenzhen Guangdong China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3998-8699","authenticated-orcid":false,"given":"Jianchun","family":"Wang","sequence":"additional","affiliation":[{"name":"Shenzhen Grubbs Institute and Department of Chemistry, Guangming Advanced Research Institute, and Guangdong Provincial Key Laboratory of Catalysis Southern University of Science and Technology  Shenzhen Guangdong 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