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High\u2010performance OSC active layers commonly comprise polymer donors and small molecule acceptors. Enhanced crystallinity, ordered molecular packing, and strong intermolecular interactions in polymer donors can improve carrier mobility and photovoltaic performance. This study introduces a new polymer, D18\u20106F, synthesized using 2\u2010(3,4,5\u2010trifluorophenyl)thiophene as an end\u2010capping unit for the high\u2010performance polymer donor D18. D18\u20106F exhibits improved intermolecular interactions, ordered molecular packing, and crystallinity, leading to better miscibility between donor and acceptor components and optimized blend film morphology. Consequently, OSC devices based on D18\u20106F achieved a power conversion efficiency of 19.45%, up from 18.47% (D18). This research offers a valuable strategy for designing high\u2010efficiency polymer donor materials.<\/jats:p>","DOI":"10.1002\/smtd.202501209","type":"journal-article","created":{"date-parts":[[2025,8,22]],"date-time":"2025-08-22T07:01:24Z","timestamp":1755846084000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Optimizing Photovoltaic Performance through Functional End\u2010Capping Units of Polymer Donor Materials"],"prefix":"10.1002","volume":"9","author":[{"given":"Chenglin","family":"Gu","sequence":"first","affiliation":[{"name":"College of Textiles &amp; Clothing Qingdao University  Qingdao 266071 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yueheng","family":"Liu","sequence":"additional","affiliation":[{"name":"College of Textiles &amp; Clothing Qingdao University  Qingdao 266071 P. R. 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