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In Y\u2010series NFAs, excessive H\u2010like core contacts may increase packing disorder, while terminal group\u2010mediated J\u2010like interactions favor electronic coupling, luminescence, and reduced nonradiative loss. Controlling the H\/J aggregation balance therefore remains a key challenge. Herein, three novel NFAs\u2014C8C8, C8\u20107R, and C8EH\u2014featuring identical conjugated backbones but systematically varied inner alkyl chains were designed to finely modulate aggregation states. Theoretical calculations and single\u2010crystal analysis show that increased inner\u2010chain steric hindrance suppresses core\u2010involved contacts (H\u2010aggregation) while favoring terminal group\u2010mediated (J\u2010aggregation) interactions. Accordingly, C8EH exhibits the strongest J\u2010preferred packing tendency and enhanced molecular ordering, supported by compact terminal contacts, redshifted absorption, faster aggregation, and refined fibrillar morphology. When fabricated with the donor D18, C8EH\u2010based OSC devices delivered an outstanding power conversion efficiency (PCE) of 20.73%, representing one of the highest values reported for additive\u2010 and annealing\u2010free OSCs with higher current and reduced energy loss. This work demonstrates that inner\u2010chain steric modulation can promote J\u2010aggregated packing and ordered molecular organization, providing an effective strategy for high\u2010performance NFAs and process\u2010simplified OSCs.<\/jats:p>","DOI":"10.1002\/adma.74902","type":"journal-article","created":{"date-parts":[[2026,9,4]],"date-time":"2026-09-04T10:23:36Z","timestamp":1788517416000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Ordered J\u2010Aggregation Directed by Inner Alkyl Chains Enables Additive\u2010 and Annealing\u2010Free Organic Solar Cells With 20.73% Efficiency"],"prefix":"10.1002","author":[{"given":"Chang","family":"Liu","sequence":"first","affiliation":[{"name":"School of Electrical Engineering &amp; College of Mechanical Engineering University of South China  Hengyang China"},{"name":"Hunan Chang\u2010rui New Energy Limited Company  Hengyang China"},{"name":"Engineering and Research Center For Integrated New Energy Photovoltaics &amp; Energy Storage Systems of Hunan Province University of South China  Hengyang Hunan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zihao","family":"Li","sequence":"additional","affiliation":[{"name":"School of Electrical Engineering &amp; College of Mechanical Engineering University of South China  Hengyang China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xingjie","family":"Mi","sequence":"additional","affiliation":[{"name":"School of Electrical Engineering &amp; College of Mechanical Engineering University of South China  Hengyang China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0393-4517","authenticated-orcid":false,"given":"Dingqin","family":"Hu","sequence":"additional","affiliation":[{"name":"Department of Mechanical Engineering City University of Hong Kong  Hong Kong 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