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In this work, it is clarified that the molecular packing of acceptor and molecule\u2010solvent interaction plays an essential role in determining the photovoltaic performance of blade\u2010coated layer\u2010by\u2010layer OSCs. It is demonstrated that the unique dimer packing feature of L8\u2010BO\u20104Cl can lead to lower excited energy (\u2206\n                    <jats:italic>E<\/jats:italic>\n                    <jats:sub>S1<\/jats:sub>\n                    ) and dominant\n                    <jats:italic>J<\/jats:italic>\n                    \u2010aggregates in the blade\u2010coated film compared to the analogs of Y6 and L8\u2010BO. Meanwhile, the weaker molecule\u2010solvent interaction between L8\u2010BO\u20104Cl and toluene is in favor of forming prominent\n                    <jats:italic>J<\/jats:italic>\n                    \u2010aggregation in blade\u2010coated film, contributing to a\u00a0more compact \u03c0\u2010stacking than Y6 and L8\u2010BO. Additionally, the blade\u2010coated D18\/L8\u2010BO\u20104Cl film shows more defined interpenetrating networks with clearer donor\u2010acceptor interfaces than D18\/Y6 and D18\/L8\u2010BO, facilitating improved charge extraction and suppressed charge recombination. As a result, the air\u2010blade\u2010coated layer\u2010by\u2010layer device based on D18\/L8\u2010BO\u20104Cl yields a remarkable power\u2010conversion efficiency (PCE) of 19.31% without any additive and post\u2010treatment, while much lower PCEs of 7.01% and 16.47% are obtained in the device based on D18\/Y6 and D18\/L8\u2010BO, respectively. This work offers an effective approach to developing highly efficient air\u2010blade\u2010coated layer\u2010by\u2010layer OSCs.\n                  <\/jats:p>","DOI":"10.1002\/adma.202502579","type":"journal-article","created":{"date-parts":[[2025,4,29]],"date-time":"2025-04-29T05:09:32Z","timestamp":1745903372000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":32,"title":["Aggregation Engineering of Toluene\u2010Processed Acceptor Layer Enables Over 19% Efficiency of Air\u2010Blade\u2010Coated Organic Solar Cells"],"prefix":"10.1002","volume":"37","author":[{"given":"Yu","family":"Ge","sequence":"first","affiliation":[{"name":"Laboratory of Advanced Optoelectronic Materials Suzhou Key Laboratory of Novel Semiconductor\u2010Optoelectronics Materials and Devices State Key Laboratory of Bioinspired Interfacial Materials Science College of Chemistry Chemical Engineering and Materials Science Soochow University  Suzhou Jiangsu 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