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However, achieving high\u2013performance as\u2013cast devices remains challenging because it demands delicate balance between donor\u2013acceptor self\u2013aggregation and miscibility. Herein, we fabricate as\u2013cast OSCs through Flory\u2013Huggins parameter (\u03c7) engineering that precisely regulates donor\u2013acceptor miscibility during solution casting. The chloroform\u2013carbon disulfide (CF:CS\n                    <jats:sub>2<\/jats:sub>\n                    ) mixed solvent, with tailored solubility and evaporation kinetics, dynamically modulates \u03c7 to form an optimized bulk heterojunction featuring desirable phase separation and a well\u2013balanced fibrillar network. This design affords efficient exciton dissociation, facilitated charge transport, and suppressed recombination in the blend. Consequently, as\u2013cast D18:L8\u2013BO device processed with the CF:CS\n                    <jats:sub>2<\/jats:sub>\n                    solvent system attained a PCE of 20.11% (certified as 19.69%) alongside enhanced photostability, representing the highest efficiency reported for as\u2013cast devices. Besides, high PCEs of 18.89% and 15.12% are achieved in thick\u2013film (300\u00a0nm) and large\u2013area (20.17 cm\n                    <jats:sup>2<\/jats:sup>\n                    ) as\u2013cast devices. Moreover, a quantitative correlation between PCE and the interaction parameter \u03c7 is established, providing a quantitative guide for narrowing the miscibility window and identifying the optimal composition. These findings validate the efficacy of \u03c7\u2013parameter\u2013mediated miscibility engineering in regulating blend phase behavior and provide a framework for advancing efficient as\u2013cast OSCs.\n                  <\/jats:p>","DOI":"10.1002\/adma.75152","type":"journal-article","created":{"date-parts":[[2026,9,27]],"date-time":"2026-09-27T07:16:48Z","timestamp":1790493408000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Over 20% Efficiency in As\u2013Cast Organic Solar Cells Enabled by Flory\u2013Huggins Parameter Engineering"],"prefix":"10.1002","author":[{"given":"Zhengqi","family":"Liu","sequence":"first","affiliation":[{"name":"College of Materials Science and Opto\u2010Electronic Technology University of Chinese Academy of Sciences  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mingyan","family":"Zhan","sequence":"additional","affiliation":[{"name":"College of Materials Science and Opto\u2010Electronic Technology University of Chinese Academy of Sciences  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yanan","family":"Wei","sequence":"additional","affiliation":[{"name":"College of Materials Science and Opto\u2010Electronic Technology University of Chinese Academy of Sciences  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0001-6322-2140","authenticated-orcid":false,"given":"Mingxu","family":"Zhou","sequence":"additional","affiliation":[{"name":"School of Physics State Key Laboratory of Crystal Materials Shandong University  Jinan Shandong P. R. 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