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However, the formation of defect\u2010free and densely packed films is often hindered by poor dispersibility, micelle\u2010like aggregation, and incomplete surface coverage. Here, we develop a cooperative dipole and anchoring strategy by pairing an asymmetric, conjugation\u2010extended phosphonic\u2010acid SAM (3\u2010BFCz) with a fluorinated quinoline\u20104\u2010carboxylic acid co\u2010adsorbate (QLCA\u2010F) to construct a bimolecular co\u2010adsorbed interface (CA). Owing to its enlarged dipole moment (2.70 D vs. 1.89 D for 2PACz), 3\u2010BFCz increases the ITO work function (WF) from 4.90 to 5.01\u00a0eV, while co\u2010adsorption with QLCA\u2010F further raises the WF to 5.07\u00a0eV and yields a more uniform, densely packed SAM layer. As a result, the CA interface mitigates interfacial energy\/charge losses, suppresses leakage and recombination, and facilitates hole extraction\/transport, delivering consistently improved device performance across multiple high\u2010efficiency photoactive layer systems: the champion PCEs are enhanced from 19.02% to 19.54% (PM6:L8\u2010BO), from 19.10% to 19.62% (D18:N3), and from 19.69% to 20.26% (D18:L8\u2010BO\u2010X). Moreover, CA markedly improves device stability, extending the\n                    <jats:italic>T<\/jats:italic>\n                    <jats:sub>80<\/jats:sub>\n                    lifetime at 60\u00b0C by 43%. This work highlights bimolecular co\u2010adsorption as a transferable route to simultaneously optimize WF tuning, interfacial assembly quality, and device stability for high\u2010efficiency OSCs.\n                  <\/jats:p>","DOI":"10.1002\/smll.73766","type":"journal-article","created":{"date-parts":[[2026,5,12]],"date-time":"2026-05-12T09:06:08Z","timestamp":1778576768000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Cooperative Dipole and Anchoring Engineering via Bimolecular Self\u2010Assembled Monolayer for Organic Solar Cells with Efficiency of 20.26%"],"prefix":"10.1002","volume":"22","author":[{"given":"Jieyang","family":"Li","sequence":"first","affiliation":[{"name":"Beijing Advanced Innovation Center for Soft Matter Science and Engineering &amp; State Key Laboratory of Organic\u2013Inorganic Composites Beijing University of Chemical Technology  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaoping","family":"Jiang","sequence":"additional","affiliation":[{"name":"Beijing Advanced Innovation Center for Soft Matter Science and Engineering &amp; State Key Laboratory of Organic\u2013Inorganic Composites Beijing University of Chemical Technology  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Erqin","family":"Guo","sequence":"additional","affiliation":[{"name":"Beijing Advanced Innovation Center for Soft Matter Science and Engineering &amp; State Key Laboratory of Organic\u2013Inorganic Composites Beijing University of Chemical Technology  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qiaomei","family":"Chen","sequence":"additional","affiliation":[{"name":"Beijing Advanced Innovation Center for Soft Matter Science and Engineering &amp; State Key Laboratory of Organic\u2013Inorganic Composites Beijing University of Chemical Technology  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hui","family":"Huang","sequence":"additional","affiliation":[{"name":"Beijing Advanced Innovation Center for Soft Matter Science and Engineering &amp; State Key Laboratory of Organic\u2013Inorganic Composites Beijing University of Chemical Technology  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zihao","family":"Gao","sequence":"additional","affiliation":[{"name":"Beijing Advanced Innovation Center for Soft Matter Science and Engineering &amp; State Key Laboratory of Organic\u2013Inorganic Composites Beijing University of Chemical Technology  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chenhui","family":"Zhang","sequence":"additional","affiliation":[{"name":"College of Chemistry and Molecular Engineering Peking University  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7329-4236","authenticated-orcid":false,"given":"Weiwei","family":"Li","sequence":"additional","affiliation":[{"name":"Beijing Advanced Innovation Center for Soft Matter Science and Engineering &amp; State Key Laboratory of Organic\u2013Inorganic Composites Beijing University of Chemical Technology  Beijing P. R. 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