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However, the high boiling points of halogen\u2010free solvents often trigger excessive pre\u2010aggregation of non\u2010fullerene acceptors (NFAs) and unfavorable phase separation, severely limiting device performance. Herein, a side\u2010chain steric engineering strategy is employed to develop a weakly crystalline NFA, TPD\u2010Y, featuring a thieno[3,4\u2010\n                    <jats:italic>c<\/jats:italic>\n                    ]pyrrole\u20104,6\u2010dione unit. The reduced crystallinity of TPD\u2010Y effectively suppresses aggregation\u2010caused quenching (ACQ), yielding a high photoluminescence quantum yield (PLQY) of 8.19% and significantly minimized non\u2010radiative voltage loss. Furthermore, TPD\u2010Y acts as a potent crystallization\u2010kinetics modulator in multi\u2010component blends with the benchmark acceptor BTP\u2010eC9. It forms an alloy phase that simultaneously promotes nucleation and inhibits excessive grain growth in non\u2010halogenated solvents, accelerating film formation while refining oversized domains. This kinetic modulation yields an optimized nanoscale morphology with enlarged interfacial areas, synergistically enhancing exciton dissociation and charge collection. Consequently, quaternary OSCs processed from a non\u2010halogenated\n                    <jats:italic>o<\/jats:italic>\n                    \u2010xylene\/carbon disulfide mixture achieve a remarkable fill factor of nearly 82% and a record power conversion efficiency exceeding 21%. This work provides a robust molecular design to overcome the efficiency bottleneck of chlorinated\u2010solvent\u2010free OSCs, marking a significant step toward the industrialization of high\u2010performance, low\u2010toxicity photovoltaics.\n                  <\/jats:p>","DOI":"10.1002\/smll.75263","type":"journal-article","created":{"date-parts":[[2026,8,14]],"date-time":"2026-08-14T05:46:56Z","timestamp":1786686416000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Taming Crystallization Kinetics via Side\u2010Chain Steric Engineering Enables Over 21% Efficiency in Non\u2010Halogenated\u2010Solvent\u2010Processed Organic Solar Cells"],"prefix":"10.1002","volume":"22","author":[{"given":"Shengxi","family":"Zhou","sequence":"first","affiliation":[{"name":"Beijing Advanced Innovation Center for Soft Matter Science and Engineering &amp; State Key Laboratory of Organic\u2010Inorganic Composites Beijing University of Chemical Technology  Beijing People's Republic of China"},{"name":"Department of Chemistry and Bioscience, Sino\u2010Danish Center for Education and Research Aalborg University  Aalborg Denmark"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7253-7136","authenticated-orcid":false,"given":"Chengyi","family":"Xiao","sequence":"additional","affiliation":[{"name":"Beijing Advanced Innovation Center for Soft Matter Science and Engineering &amp; State Key Laboratory of Organic\u2010Inorganic Composites Beijing University of Chemical Technology  Beijing People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mengdi","family":"Li","sequence":"additional","affiliation":[{"name":"Beijing Advanced Innovation Center for Soft Matter Science and Engineering &amp; State Key Laboratory of Organic\u2010Inorganic Composites Beijing University of Chemical Technology  Beijing People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bo","family":"Wang","sequence":"additional","affiliation":[{"name":"Beijing Advanced Innovation Center for Soft Matter Science and Engineering &amp; State Key Laboratory of Organic\u2010Inorganic Composites Beijing University of Chemical Technology  Beijing People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xucong","family":"Liu","sequence":"additional","affiliation":[{"name":"Beijing Advanced Innovation Center for Soft Matter Science and Engineering &amp; State Key Laboratory of Organic\u2010Inorganic Composites Beijing University of Chemical Technology  Beijing People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0003-1618-8618","authenticated-orcid":false,"given":"Yao","family":"Li","sequence":"additional","affiliation":[{"name":"Advanced Materials Thrust, Function Hub The Hong Kong University of Science and Technology (Guangzhou)  Guangzhou People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9674-2903","authenticated-orcid":false,"given":"Jiaying","family":"Wu","sequence":"additional","affiliation":[{"name":"Advanced Materials Thrust, Function Hub The Hong Kong University of Science and Technology (Guangzhou)  Guangzhou People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Donghong","family":"Yu","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Bioscience, Sino\u2010Danish Center for Education and Research Aalborg University  Aalborg Denmark"},{"name":"Sino\u2010Danish Center for Education and Research  Aarhus Denmark"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4942-3771","authenticated-orcid":false,"given":"Ergang","family":"Wang","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Chemical Engineering Chalmers University of Technology  G\u00f6teborg Sweden"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7329-4236","authenticated-orcid":false,"given":"Weiwei","family":"Li","sequence":"additional","affiliation":[{"name":"Beijing Advanced Innovation Center for Soft Matter Science and Engineering &amp; 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