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Achieving precise control over NFA aggregation during film formation is thus essential to realize optimal molecular orientation and phase separation. Herein, we propose an unsaturated vinyl branching (UVB) strategy that enables synergistic morphology control through the concurrent minimization of steric hindrance and enhancement of non\u2010covalent interactions. By incorporating UVB units into the inner side chains of the Y6\u2010OD backbone, we create a novel acceptor, BTP\u2010vinyl, which demonstrates optimized aggregation kinetics and facilitates compact 3D molecular packing. When blended with polymer donor D18, the BTP\u2010vinyl\u2010based system exhibits retarded crystallization, optimized domain size, and highly ordered face\u2010on orientation, collectively promoting efficient exciton dissociation and charge transport. Consequently, OSCs based on BTP\u2010vinyl display significantly reduced energetic disorder and suppressed non\u2010radiative energy loss compared to Y6\u2010OD\u2010based devices. The binary devices achieve a remarkable power conversion efficiency (PCE) of 19.6%, substantially outperforming the Y6\u2010OD\u2010based devices (18.1%). Furthermore, ternary devices incorporating L8\u2010BO attain a champion PCE of 20.06%, crossing the significant 20% threshold. This work establishes UVB as an effective molecular\u2010design paradigm for achieving ideal blend morphology through precise aggregation control in high\u2010performance OSCs.<\/jats:p>","DOI":"10.1002\/adma.202520692","type":"journal-article","created":{"date-parts":[[2025,12,26]],"date-time":"2025-12-26T13:58:54Z","timestamp":1766757534000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":15,"title":["Unsaturated Vinyl Branching: A Molecular\u2010Tailoring Strategy for Synergistic Stacking Regulation and Energy\u2010Loss Suppression Toward 20%\u2010Efficiency Organic Solar Cells"],"prefix":"10.1002","volume":"38","author":[{"given":"Ling","family":"Li","sequence":"first","affiliation":[{"name":"Guangxi Colleges and Universities Key Laboratory of Surface and Interface Electrochemistry, Guangxi Key Laboratory of Electrochemical and Magneto\u2010chemical Functional Materials, College of Chemistry and Bioengineering Guilin University of Technology Guilin Guangxi 541006 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wenzhao","family":"Xiong","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Advanced Fibers and Materials, College of Materials Science and Engineering Donghua University Shanghai 201620 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yanyan","family":"Zhang","sequence":"additional","affiliation":[{"name":"Guangxi Colleges and Universities Key Laboratory of Surface and Interface Electrochemistry, Guangxi Key Laboratory of Electrochemical and Magneto\u2010chemical Functional Materials, College of Chemistry and Bioengineering Guilin University of Technology Guilin Guangxi 541006 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhibo","family":"Wang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Advanced Fibers and Materials, College of Materials Science and Engineering Donghua University Shanghai 201620 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Junyin","family":"Dong","sequence":"additional","affiliation":[{"name":"Function Hub, Advanced Materials Thrust The Hong Kong University of Science and Technology Guangzhou Guangdong 511400 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shenbo","family":"Zhu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Advanced Fibers and Materials, College of Materials Science and Engineering Donghua University Shanghai 201620 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xueming","family":"Li","sequence":"additional","affiliation":[{"name":"Guangxi Colleges and Universities Key Laboratory of Surface and Interface Electrochemistry, Guangxi Key Laboratory of Electrochemical and Magneto\u2010chemical Functional Materials, College of Chemistry and Bioengineering Guilin University of Technology Guilin Guangxi 541006 P.R. 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