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Additive engineering can effectively modulate film morphology, but it always relies on halogen\u2010based interactions with photoactive materials, compromising environmental sustainability. Herein, we developed three novel halogen\u2010free additives, namely cyclohexylbenzene (ChB), 1,4\u2010dicyclohexylbenzene (DChB), and 1,3,5\u2010tricyclohexylbenzene (TChB), which are benzene derivatives substituted with different numbers of cyclohexyl groups. These additives enable precise regulation of molecular packing and crystallization through distinct steric hindrance effects and additive\u2013acceptor interactions. Both theoretical and experimental investigations reveal that the bulky cyclohexyl groups preferentially adsorb onto the terminal units of L8\u2010BO, creating steric spacers that effectively suppress excessive aggregation during the halogen\u2010free solvent processing. Moreover, the additives serve as kinetic mediators during spin\u2010coating to promote compact terminal packing of L8\u2010BO, while their subsequent thermal volatilization further promotes well\u2010ordered long\u2010range crystallinity. The resulting microstructure significantly enhances charge utilization, enabling D18:L8\u2010BO OSCs to achieve a record\u2010breaking efficiency of 20.50% with improved operational stability. This work underscores the unique advantage of halogen\u2010free additives in selectively modulating molecular aggregation, enabling dual eco\u2010friendly fabrication and paving the way for commercialization of high\u2010performance organic photovoltaics.<\/jats:p>","DOI":"10.1002\/adma.74819","type":"journal-article","created":{"date-parts":[[2026,8,26]],"date-time":"2026-08-26T14:59:49Z","timestamp":1787756389000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Halogen\u2010Free Solvent and Additive\u2010Processed Organic Solar Cells Achieving 20.50% Binary Efficiency"],"prefix":"10.1002","volume":"38","author":[{"given":"Ziwei","family":"Zhang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Bioinspired Interfacial Materials Science, International Research Center for Carbon Neutralization, Hangzhou International Innovation Institute Beihang University  Hangzhou P. R. 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