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However, conventional SD methods often face challenges such as interfacial erosion and disordered crystallization, which limit further efficiency improvements. Herein, we report a novel thermally annealed donor\u2010assisted sequential deposition (TD\u2010SD) strategy aimed at modulating the film\u2010formation kinetics during the SD process. By pre\u2010annealing the donor layer, an ordered donor molecular packing is formed. Moreover, the thermal effect provided by the donor accelerated the aggregation kinetics of the acceptor, which helps mitigate the erosion of the donor by the acceptor. Therefore, a more pronounced vertical gradient distribution is formed. Such an optimized morphology promotes exciton dissociation and charge transport. Consequently, the devices based on TD\u2010SD strategy exhibit superior photovoltaic performance, with the champion device achieving a power conversion efficiency (PCE) of 20.35%, up from 18.65% for the D18\u2010Cl\/L8\u2010BO device. Notably, the strategy also enabled a high PCE of 20.81% (certified as 20.25%) in the D18\u2010Cl\/L8\u2010BO:BTP\u2010eC9 system, placing it among the top\u2010performing OSCs. This study offers a practical route for precisely controlling the morphology of OSCs processed via SD processing.<\/jats:p>","DOI":"10.1002\/adma.74911","type":"journal-article","created":{"date-parts":[[2026,9,4]],"date-time":"2026-09-04T10:28:49Z","timestamp":1788517729000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Kinetic Management of Vertical Phase Separation via Thermal Annealed Donor\u2010Assisted Sequential Deposition Enables 20.81% Efficiency in Organic Solar Cells"],"prefix":"10.1002","author":[{"given":"Shizhao","family":"Liu","sequence":"first","affiliation":[{"name":"Shandong Provincial Key Laboratory for Science of Material Creation and Energy Conversion Science Center for Material Creation and Energy Conversion Institute of Frontier Chemistry School of Chemistry and Chemical Engineering Shandong University  Qingdao 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