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This trade\u2010off remains a key limitation to further improving photovoltaic efficiency. Here, we probe this dilemma through linkage\u2010topology engineering by incorporating highly crystalline and luminescent 3,6\u2010dichlorocarbazole units into SMA backbones. Through systematic linker variation, we tune acceptor self\u2010aggregation and donor\/acceptor intermolecular interactions, thereby mitigating this intrinsic trade\u2010off. By modulating molecular linkage mode from a direct C\u2500N connection (CHC\u20101) to a flexible methylene bridge (CHC\u20102) and a rigid carbonyl bridge (CHC\u20103), we achieve orthogonal control over acceptor aggregation and donor\/acceptor interfacial coupling. Notably, carbonyl\u2010bridged CHC\u20103 shows the weakest acceptor self\u2010association, but the strongest donor\/acceptor coupling with PM6. This combination suppresses charge\u2010transfer\u2010state nonradiative recombination and optimizes film\u2010forming kinetics, leading to an improved vertical composition gradient and a refined surface morphology. Consequently, CHC\u20103\u2010based binary and ternary devices achieve PCEs of 18.79% and 20.58%, respectively, with a markedly reduced \u0394\n                    <jats:italic>E<\/jats:italic>\n                    <jats:sub>nrad<\/jats:sub>\n                    of 0.204\u00a0eV. This work establishes linkage\u2010topology engineering as an effective strategy for balancing luminescence efficiency, charge transport, and morphology in sterically modified SMAs.\n                  <\/jats:p>","DOI":"10.1002\/anie.6595038","type":"journal-article","created":{"date-parts":[[2026,9,4]],"date-time":"2026-09-04T08:52:28Z","timestamp":1788511948000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Linker\u2010Mediated Trade\u2010Off Between Acceptor Aggregation and Donor\u2013Acceptor Mixing Enables Organic Solar Cells With Efficiencies Exceeding 20.5%"],"prefix":"10.1002","volume":"65","author":[{"given":"Jie","family":"Wang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Elemento\u2010Organic Chemistry Frontiers Science Center for New Organic Matter Key Laboratory of Functional Polymer Materials Nankai University  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wendi","family":"Shi","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Elemento\u2010Organic Chemistry Frontiers Science Center for New Organic Matter Key Laboratory of Functional Polymer Materials Nankai University  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zezhou","family":"Liang","sequence":"additional","affiliation":[{"name":"Key Laboratory of Flexible Optoelectronic Materials and Technology (Ministry of Education), School of Optoelectronic Materials &amp; Technology Jianghan University  Wuhan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiong","family":"Yang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Elemento\u2010Organic Chemistry Frontiers Science Center for New Organic Matter Key Laboratory of Functional Polymer Materials Nankai University  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Huanhuan","family":"Gao","sequence":"additional","affiliation":[{"name":"Shandong Key Laboratory of Functional\u2010Structural Integrated Ceramics Discipline and Technology Center for High Temperature Functional Ceramics School of Materials Science and Engineering Shandong University of Technology  Zibo Shandong China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wenkai","family":"Zhao","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering National Institute for Advanced Materials Nankai University  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1826-3736","authenticated-orcid":false,"given":"Guankui","family":"Long","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering National Institute for Advanced Materials Nankai University  Tianjin 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