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Inspired by natural Mo\u2010containing enzymes, we develop Mo\u2010on\u2010Cu nanosheets (Mo\u2010Cu NSs) via electrochemical reduction of CuO NSs followed by Mo deposition through electron\u2010beam evaporation. The bioinspired Mo\u2010Cu NSs deliver outstanding activity, achieving a urea partial current density of 2.39\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    with a Faradaic efficiency (FE) of 52% at \u22120.2\u00a0V versus RHE, and a methanol FE of 65% at \u22120.5\u00a0V versus RHE, ranking among the most efficient electrocatalysts for co\u2010synthesis of urea and methanol. In situ electrochemical characterizations and density functional theory (DFT) calculations reveal that interfacial electron redistribution between electron\u2010rich Cu and electron\u2010deficient Mo optimizes intermediate conversion pathways, thereby enabling potential\u2010dependent product selectivity. Specifically, *CO\n                    <jats:sub>2<\/jats:sub>\n                    and *NOH coupling accounts for urea formation, while *NO intermediates promote methanol production. This study not only provides a new electrocatalyst for highly efficient urea and methanol electrosynthesis but also can guide the design of other electrocatalysts for high\u2010value chemicals.\n                  <\/jats:p>","DOI":"10.1002\/anie.202520792","type":"journal-article","created":{"date-parts":[[2026,2,6]],"date-time":"2026-02-06T09:20:53Z","timestamp":1770369653000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":7,"title":["Bioinspired Mo\u2010on\u2010Cu Nanosheets Enable Potential\u2010Dependent Electrosynthesis of Urea and Methanol via Interfacial Electron Redistribution"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0009-0006-4789-7865","authenticated-orcid":false,"given":"Liming","family":"Deng","sequence":"first","affiliation":[{"name":"Zhejiang Key Laboratory of Functional Ionic Membrane Materials and Technology for Hydrogen Production Shaoxing University  Shaoxing 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