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Homogeneous redox mediators (RMs) in organic electrosynthesis are effective platforms for this purpose. However, understanding the RM's electronic structure under operational conditions, electron transport processes at the electrode surface, and substrate adsorption\u2010desorption dynamics remains challenging. Here, we synthesized a Cu single\u2010atom catalyst (SAC, named Cu\u2500N\u2500P@NC) with a CuN\n                    <jats:sub>3<\/jats:sub>\n                    P\n                    <jats:sub>1<\/jats:sub>\n                    micro\u2010coordination structure, employing it as a unique cathode redox mediator. Introducing phosphine atoms into the coordination system allowed modulation of the SAC's electronic metal\u2010support interaction, optimizing catalyst\u2010substrate adsorption\u2010desorption dynamics and accelerating electrochemical reactions. Utilizing the heterogeneous SAC strategy, we achieved a novel electro\u2010reduction coupling ring\u2010opening reaction of inert quinazolinone frameworks. The Cu\u2010SAC exhibited exceptionally high catalytic activity and substrate compatibility, operating smoothly at gram\u2010scale production. Additionally, we applied the SAC to modify 11 natural product molecules. Integrating micro\u2010coordination environment regulation and theoretical adsorption models elucidated the significant influence of electrode\u2010RMs\u2010substrate interactions on reaction kinetics and catalytic efficiency\u2010a feat challenging for homogeneous RMs. This approach offers a novel pathway for advancing efficient organic electrosynthesis reactions and provides critical insights for mechanistic studies.\n                  <\/jats:p>","DOI":"10.1002\/anie.202505085","type":"journal-article","created":{"date-parts":[[2025,3,19]],"date-time":"2025-03-19T23:33:16Z","timestamp":1742427196000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":39,"title":["Phosphorus\u2010Doped Single Atom Copper Catalyst as a Redox Mediator in the Cathodic Reduction of Quinazolinones"],"prefix":"10.1002","volume":"64","author":[{"given":"Xin\u2010Yu","family":"Wang","sequence":"first","affiliation":[{"name":"Department of Chemistry 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