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While lattice strain engineering can modulate catalytic performance by altering electronic structures, a major challenge is the lack of a clear mechanistic understanding connecting the induced strain to the activity enhancement. Herein, by precisely engineering lattice strain in an atomically integrated catalytic system, we establish a definitive intrinsic structure\u2010activity relationship, moving beyond conventional correlations with apparent properties. Combined experimental and theoretical investigations demonstrate that compressive strain effectively modulates the electronic structure of the Cu d\u2010orbital and the local electronic states of oxygen vacancies, thereby enhancing the cooperation within the Lewis acid\u2013base pairs. This mechanism facilitates CO\n                    <jats:sub>2<\/jats:sub>\n                    adsorption and activation, stabilizes the key\n                    <jats:sup>*<\/jats:sup>\n                    HCOO intermediate, and significantly lowers the reaction energy barrier. Consequently, the catalyst exhibits high formate Faradaic efficiency (&gt;95%) over a broad current density range (\u2212100 to \u2212700 mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    ), achieving 96.1% at \u2212576.8 mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    . This research not only elucidates the synergistic Lewis acid\u2010base catalytic mechanism at the molecular level but also provides universal design principles for the sustainable electro\u2010synthesis of value\u2010added formate.\n                  <\/jats:p>","DOI":"10.1002\/adma.202519866","type":"journal-article","created":{"date-parts":[[2025,12,18]],"date-time":"2025-12-18T09:01:59Z","timestamp":1766048519000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":12,"title":["Designing Synergistic Lewis Acid\u2010Base Pairs in Compressed Bismuth\u2010Copper Oxide for Selective CO\n                    <sub>2<\/sub>\n                    \u2010to\u2010Formate Electrosynthesis"],"prefix":"10.1002","volume":"38","author":[{"given":"Yi","family":"Cheng","sequence":"first","affiliation":[{"name":"Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of China  Chengdu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lijuan","family":"Yang","sequence":"additional","affiliation":[{"name":"Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of China  Chengdu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaoli","family":"Zhao","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Xihua University  Chengdu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lulu","family":"Li","sequence":"additional","affiliation":[{"name":"Institute of Chemical Research of Catalonia (ICIQ\u2010CERCA) The Barcelona Institute of Science and Technology (BIST)  Tarragona Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jian","family":"Yang","sequence":"additional","affiliation":[{"name":"National Engineering Research Center of Electromagnetic Radiation Control Materials University of Electronic Science and Technology of China  Chengdu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tao","family":"Liu","sequence":"additional","affiliation":[{"name":"National Engineering Research Center of Electromagnetic Radiation Control Materials University of Electronic Science and Technology of China  Chengdu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Feng","family":"Li","sequence":"additional","affiliation":[{"name":"Laboratory of Advanced Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Fudan University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9188-4619","authenticated-orcid":false,"given":"Ming","family":"Huang","sequence":"additional","affiliation":[{"name":"Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of China  Chengdu 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