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Here, we develop a co-assembled multilayered SAM (coSAMu) strategy that combines two SAM molecules, 2PACz and 2Cl-4PACz, with distinct dipoles and steric configurations through blend casting and sequential casting. Photoelectron spectroscopy, X-ray analysis, and molecular simulations support a layered structure in which a chemisorbed, 2PACz-rich bottom layer primarily sets the indium tin oxide (ITO) work function, while a 2Cl-4PACz-rich upper\u00a0layer fills interfacial voids, improves molecular packing, and passivates defects. Consistent with this picture, coSAMu promotes a more favorable vertical composition near the ITO surface and suppresses trap-assisted recombination, enabling more efficient charge extraction and collection. Consequently, a\u00a0representative D18:L8-BO OSC incorporating the sequential-cast coSAMu HTL achieves a power conversion efficiency of 20.1% (0.042 cm\n                    <jats:sup>2<\/jats:sup>\n                    ), outperforming pristine 2PACz. Importantly, when scaled to a 17.14 cm\n                    <jats:sup>2<\/jats:sup>\n                    mini-module (six serially connected subcells), coSAMu delivers 17.0% efficiency versus 12.2% for the 2PACz control. This work demonstrates controlled multilayer co-assembly as an effective strategy for scalable OSC interface engineering that is broadly applicable to multiple donor\u2013acceptor systems.\n                  <\/jats:p>","DOI":"10.1007\/s40820-026-02325-2","type":"journal-article","created":{"date-parts":[[2026,8,10]],"date-time":"2026-08-10T07:08:43Z","timestamp":1786345723000},"update-policy":"https:\/\/doi.org\/10.1007\/springer_crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Layered Defect-Filling co-Assembled Carbazole-Based SAMs Deliver 20% Organic Solar Cells and 17% Mini-Modules"],"prefix":"10.1007","volume":"19","author":[{"given":"Jingnan","family":"Wu","sequence":"first","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fengbo","family":"Sun","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Leandro R.","family":"Franco","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qiaonan","family":"Chen","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinxin","family":"Xia","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ruike","family":"Zhou","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhuang","family":"Li","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mateus","family":"Bergami","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Pablo Hermosilla","family":"Fernandez","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"C. 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