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Herein, we demonstrate that fluorine positional isomerism serves as a precise molecular handle to reconcile this conflict by modulating aggregation behaviors. Through regulating fluorine substitution from alkoxy ortho\u2010 (PFo) to meta\u2010 (PFm) and para\u2010 (PFp) positions, a distinct transition from J\u2010aggregation to H\u2010dominant aggregation is achieved. Contrary to the conventional preference for J\u2010aggregates, the H\u2010aggregated PFp achieves superior photovoltaic performance in this BDF\u2010based polymer system, driven by the synergistic effects of HOMO stabilization, optimized packing, and matched interfacial energetics. Comprehensive dynamical studies, including vibronic analysis and transient absorption (TA) spectroscopy, reveal that H\u2010aggregation maximizes \u03c0\u2013\u03c0 orbital overlap and optimizes phase separation, thereby suppressing non\u2010radiative recombination and accelerating ultrafast charge transfer. Consequently, PFp\u2010based binary devices deliver a champion efficiency of 18.54%. Furthermore, demonstrating the universality of this strategy, PFp acts as a potent morphology regulator in ternary blends, boosting the efficiency to an impressive 19.77%. This work establishes fluorine positional isomerism as a precise molecular handle to guide H\u2010aggregation, synergistically optimizing energy levels and interfacial miscibility, offering an effective design strategy for high\u2010performance semicrystalline polymer donors.<\/jats:p>","DOI":"10.1002\/smll.74571","type":"journal-article","created":{"date-parts":[[2026,7,16]],"date-time":"2026-07-16T09:36:57Z","timestamp":1784194617000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Fluorine Positional Isomerism Enables H\u2010Aggregation for High\u2010Performance Semicrystalline Polymer Donors in Organic Solar Cells"],"prefix":"10.1002","volume":"22","author":[{"given":"Shisong","family":"Sun","sequence":"first","affiliation":[{"name":"School of Chemistry Beihang University  Beijing People's Republic of China"},{"name":"State Key Laboratory of Bioinspired Interfacial Materials Science, Bioinspired Science 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