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Here, an innovative strategy of active layer pre\u2010solidification by liquid nitrogen freezing process is proposed to accelerate molecular precipitation and crystallization, and therefore suppress the excessive phase separation, as demonstrated by PiFM and GISAXs results. Moreover, pre\u2010solidification process allows more solvents to carry acceptor molecules for an orderly upward migration during rapid volatilization, facilitating an ideal longitudinal gradient arrangement of photovoltaic materials that is favorable for charge transport and extraction. Consequently, PM6:L8BO\u2010X:BO\u20108F OSCs fabricate with <jats:italic>o<\/jats:italic>\u2010xylene yielded a record efficiency of 20.38%, which is comparable to 20.56% for chloroform\u2010processed devices. The inconspicuous efficiency gaps are observed in various photovoltaic materials by using green solvents, proving the outstanding universality. In addition, the pre\u2010solidification process effectively inhibits the coffee\u2010ring effect in large\u2010area active layer films and boosts the OSC modules to an exciting 17.06% efficiency. This work virtually eliminates the photovoltaic performance losses caused by green solvents, and charts a sustainable avenue to large\u2010scale commercialization of organic photovoltaics.<\/jats:p>","DOI":"10.1002\/adma.202503510","type":"journal-article","created":{"date-parts":[[2025,5,30]],"date-time":"2025-05-30T04:55:57Z","timestamp":1748580957000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":34,"title":["Green Solvent\u2010Processed Organic Solar Cells Approaching 20.4% Efficiency via Active Layer Pre\u2010Solidification"],"prefix":"10.1002","volume":"37","author":[{"given":"Xiaopeng","family":"Duan","sequence":"first","affiliation":[{"name":"Hangzhou International Innovation Institute Beihang University  Hangzhou 311115 P. R. China"},{"name":"School of Chemistry Beihang University  Beijing 100191 P. R. 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