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These side chains influenced significantly molecular planarity, packing and film morphology, which are critical for device performance. BTP\u2010C6 exhibits optimal molecular packing and fibril network morphology, enabling efficient exciton dissociation, charge transport and balanced carrier mobilities, finally achieving PCEs of 19.28% and 19.62% with chloroform\u2010 and toluene\u2010cast acceptor layers, respectively. BTP\u2010C8 featuring enhanced planarity (dihedral angle 8.27\u00b0) showed the loosest packing (packing coefficient 49.6%) due to the increased steric hindrance of side chains, limiting intermolecular charge transport. Conversely, BTP\u2010C12 formed a high crystalline and tightly packed 3D network but suffered from reduced intramolecular charge transfer caused by severe molecular distortion (dihedral angle 27.27\u00b0). The findings in this work underscore the critical role of side\u2010chain engineering in governing molecular packing and morphology, offering a systematic understanding of the relationships between steric hindrance, crystallinity and device performance, while providing a rational design strategy for next\u2010generation NFAs to advance high\u2010performance LBL\u2010OSCs.<\/jats:p>","DOI":"10.1002\/smll.202500602","type":"journal-article","created":{"date-parts":[[2025,4,14]],"date-time":"2025-04-14T01:54:16Z","timestamp":1744595656000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":14,"title":["Different Sized Cycloalkyl Chains on Non\u2010Fullerene Acceptors Enhance Molecular Packing, Film Morphology and Charge Transport for 19.62% Efficiency Organic Solar Cells"],"prefix":"10.1002","volume":"21","author":[{"given":"Yu","family":"Chen","sequence":"first","affiliation":[{"name":"School of Chemical Engineering and State Key Laboratory of Polymer Materials Engineering Sichuan University  Chengdu 610065 P. 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