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However, solution\u2010processed SAMs suffer from poor surface coverage and inadequate chemical anchoring on conducting substrates, especially for flexible substrates with high roughness, compromising the charge transport efficiency and device stability. Herein, we introduce thermal evaporation for depositing carbazole\u2010phosphonic SAM films and establish the correlations between molecular configurations and surface properties. Vacuum\u2010evaporated SAMs exhibit enhanced substrate coverage and surface wettability compared to solution\u2010processed counterparts through the regulated molecular packing. The increased surface energy of vacuum\u2010evaporated SAM films accelerates perovskite nucleation kinetics, balances growth rates across the films, and optimizes interfacial contact quality. Molecular configuration tailoring in the SAM backbones further refines the morphological quality and energetic alignment at the buried interface, thus promoting efficient charge transport and reduced non\u2010radiative recombination loss. As a result, the optimized devices using vacuum\u2010evaporated SAM films achieve an impressive power conversion efficiency (PCE) of 25.47% (certified 25.38%), among the highest PCEs reported for F\u2010PSCs. Furthermore, the optimized devices demonstrate enhanced mechanical durability and operational stability, underscoring a practical methodology route toward efficient and stable F\u2010PSCs.<\/jats:p>","DOI":"10.1002\/anie.202511317","type":"journal-article","created":{"date-parts":[[2025,12,4]],"date-time":"2025-12-04T06:42:07Z","timestamp":1764830527000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":13,"title":["Beyond Solution Processing: Vacuum Evaporation of Carbazole\u2010Phosphonic Self\u2010Assembled Molecules Enables Flexible Perovskite Solar Cells with &gt;25.4% Efficiency"],"prefix":"10.1002","volume":"65","author":[{"given":"Zheng","family":"Zhang","sequence":"first","affiliation":[{"name":"Key Laboratory of Applied Surface and Colloid Chemistry, National Ministry of Education; Shaanxi Key Laboratory for Advanced Energy Devices; Shaanxi Engineering Lab for Advanced Energy Technology; School of Materials Science and 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