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However, their power conversion efficiency (PCE) has long been behind that of the corresponding devices with small molecular acceptors. This is due to the precise chemical structure modulation of polymer acceptors (PAs), enabling relatively coplanar conformation and ordered molecular stacking and thus achieving ideal morphology, which remains critically challenging. Herein, in this work, we have designed two biaxial conjugate extension PAs, with various side chain\/terminal substituents to control their intermolecular non\u2010covalent interactions, thereby optimizing aggregation behavior and microstructural orientation of polymer assemblies. It was found that the alkoxy\u2010functionalized PQxO\u2010IT facilitates stronger intermolecular interactions and tighter \u03c0\u2010\u03c0 stacking. Furthermore, the PQx\u2010FT:PQxO\u2010IT composite promoted charge carrier mobility and charge transport, while effectively suppressing non\u2010radiative decay pathways. Consequently, the corresponding ternary device achieved the highest PCE of 20.29% (certified as 20.03%) for the APSC systems so far. Furthermore, the tight and ordered molecular packing endowed the flexible device with a PCE of 18.93% and remarkable durability during continuous bending tests. This study demonstrates a precise structure modulation strategy that offers a viable materials design pathway for high\u2010performance flexible photovoltaics.<\/jats:p>","DOI":"10.1002\/anie.5004335","type":"journal-article","created":{"date-parts":[[2026,6,3]],"date-time":"2026-06-03T07:00:47Z","timestamp":1780470047000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Precise Structure Regulation Induced Morphological Ordering Enables All\u2010Polymer Solar Cells With 20.29% Efficiency and Extreme Mechanical Robustness"],"prefix":"10.1002","volume":"65","author":[{"given":"Huanhuan","family":"Gao","sequence":"first","affiliation":[{"name":"School of Materials Science and Engineering Shandong Key Laboratory of Functional\u2010Structural Integrated Ceramics Discipline and Technology Center for High Temperature Functional Ceramics Shandong University of Technology  Zibo China"},{"name":"State Key Laboratory and 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