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While A\u2010D\u2010A\u2032\u2010D\u2010A\u2010type acceptors have improved efficiency by forming favorable 3D network packing, strategies to further enhance crystallinity without causing detrimental over\u2010aggregation are scarce. Herein, we report a distinctive non\u2010fullerene acceptor (NFA) congener, BrTh\u20102Cl, via a molecular fusion strategy. This design ingeniously integrates a highly crystalline brominated\u2010thiophene unit with a chlorinated phenyl group onto the central core, engineering a highly effective terminal functionality that can effectively modulate molecular packing without over\u2010aggregation. In addition, the blue\u2010shifted absorption of BrTh\u20102Cl caused by weak electron\u2010withdrawing of thiophene terminal group without malononitrile achieves complementary advantages with light harvest of L8\u2010BO. The incorporation of BrTh\u20102Cl into a D18\u2010Cl: L8\u2010BO host blend enhances film ordering and electron mobility for higher current, while simultaneously suppressing non\u2010radiative energy loss. Consequently, the adjusted OSC achieves a remarkable power\u2010conversion efficiency (PCE) of 20.82% (certified 20.34%), a significant increase from the 19.03% of the binary device, accompanied by concurrent improvements in both short\u2010circuit current density and open\u2010circuit voltage. This work provides an effective molecular fusion strategy by terminal groups to refine molecular packing and propel the photovoltaic performance of OSCs.<\/jats:p>","DOI":"10.1002\/adma.202521440","type":"journal-article","created":{"date-parts":[[2026,1,28]],"date-time":"2026-01-28T09:30:47Z","timestamp":1769592647000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Fusion Strategy Toward Highly Crystalline Non\u2010Fullerene Acceptor Enables Simultaneously Enhanced Current and Voltage in Organic Solar Cells"],"prefix":"10.1002","volume":"38","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-9478-9230","authenticated-orcid":false,"given":"Zhenye","family":"Li","sequence":"first","affiliation":[{"name":"School of Electrical Engineering &amp; College of Mechanical Engineering University of South China  Hengyang China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rujin","family":"Zhou","sequence":"additional","affiliation":[{"name":"School of Electrical Engineering &amp; College of Mechanical Engineering University of South China  Hengyang China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Huanyan","family":"Jiang","sequence":"additional","affiliation":[{"name":"School of Electrical Engineering &amp; College of Mechanical Engineering University of South China  Hengyang China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Menglong","family":"He","sequence":"additional","affiliation":[{"name":"School of Electrical Engineering &amp; College of Mechanical Engineering University of South China  Hengyang China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Siqi","family":"Fan","sequence":"additional","affiliation":[{"name":"School of Electrical Engineering &amp; College of Mechanical Engineering University of South China  Hengyang China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yixin","family":"Zuo","sequence":"additional","affiliation":[{"name":"School of Electrical Engineering &amp; College of Mechanical Engineering University of South China  Hengyang China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yufei","family":"Wang","sequence":"additional","affiliation":[{"name":"College of New Materials and New Energies Shenzhen Technology University  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuang","family":"Fu","sequence":"additional","affiliation":[{"name":"Department of Physics The Chinese University of Hong Kong New Territories  Hong Kong SAR China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qingqi","family":"Song","sequence":"additional","affiliation":[{"name":"Dongguan Key Laboratory of Interdisciplinary Science For Advanced Materials and Large\u2010Scale Scientific Facilities, School of Physical Sciences Great Bay University  Dongguan Guangdong P. 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