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Imperfections in the crystalline phases result in significant trap\u2010assisted recombination, which emerges as a critical factor limiting the fill factor (FF) of organic solar cells (OSCs). Herein, a method is introduced for precise regulation of the acceptor crystallinity, utilizing a novel upper\u2010layer acceptor processing solvent, trichloroethylene (TCE), to improve the state and vertical morphology of the active layer. The TCE solvent synergistically optimizes intermolecular interactions among acceptor molecules and balances the film\u2010forming process, thereby increasing the proportion of transport phases and forming high\u2010speed channels for electron transport, which subsequently reduces trap\u2010assisted charge recombination. As a result, the photovoltaic efficiency of binary organic solar cells reaches 20.05%. More importantly, an unprecedented FF of 83.0% is obtained, representing the highest FF value for OSCs. This facile and effective approach offers a promising means for constructing efficient charge transport networks and fabricating high\u2010efficiency and morphologically stable OSCs.<\/jats:p>","DOI":"10.1002\/adma.202501243","type":"journal-article","created":{"date-parts":[[2025,4,7]],"date-time":"2025-04-07T14:11:15Z","timestamp":1744035075000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":106,"title":["Acceptor Crystallinity Engineering Enables &gt;20% Efficiency Binary Organic Solar Cells with 83.0% Fill Factor"],"prefix":"10.1002","volume":"37","author":[{"given":"Jiawei","family":"Deng","sequence":"first","affiliation":[{"name":"Hangzhou International Innovation Institute Beihang University  Hangzhou 311115 P. R. 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