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Herein, we report a novel strategy for efficient C\u2500S bond formation through in situ modulation of frustrated Lewis acid\u2010base pairs within a copper\u2010based metal\u2010organic framework (CuBDC\u2010XN). By precisely engineering electron\u2010deficient Cu Lewis acid sites and electron\u2010rich XN\u2010functionalized Lewis base sites, this bifunctional catalyst enables the synergistic co\u2010reduction of SO\n                    <jats:sub>3<\/jats:sub>\n                    <jats:sup>2\u2212<\/jats:sup>\n                    and CO\n                    <jats:sub>2<\/jats:sub>\n                    into methanesulfonate (MS) at ambient conditions with a Faradaic efficiency of 13.77% (\u22120.78\u00a0V versus RHE). Mechanistic studies reveal that the frustrated Lewis pairs selectively stabilize key intermediates (*CHO and SO\n                    <jats:sub>3<\/jats:sub>\n                    <jats:sup>2\u2212<\/jats:sup>\n                    ) via electrostatic interactions, facilitating nucleophilic attack and C\u2500S coupling with a reduced energy barrier (0.48\u00a0eV). In situ spectroscopic analyses and DFT calculations further elucidate the dynamic adsorption\u2010configuration regulation and intermediate evolution pathway. This work not only establishes a molecular\u2010level understanding of cooperative Lewis acid\u2010base catalysis but also provides a universal design principle for the sustainable electrosynthesis of value\u2010added organosulfur compounds.\n                  <\/jats:p>","DOI":"10.1002\/anie.202509851","type":"journal-article","created":{"date-parts":[[2025,6,21]],"date-time":"2025-06-21T04:38:21Z","timestamp":1750480701000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":18,"title":["Electrocatalytic C\u2500S Cross\u2010Coupling via Engineered Frustrated Lewis Acid\u2010Base Pairs for High\u2010Efficiency Methanesulfonate Synthesis"],"prefix":"10.1002","volume":"64","author":[{"given":"Yuhang","family":"Gao","sequence":"first","affiliation":[{"name":"Key Laboratory of Photochemistry Institute of Chemistry Chinese Academy of Sciences  Beijing 100190 P.R. 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