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Using dual\u2010side in situ photoluminescence, we overturn the conventional top\u2013down model by revealing simultaneous nucleation at both gas\u2013liquid and liquid\u2013solid interfaces during antisolvent\u2010assisted solution processing, but find that outward solvent evaporation delays \u03b1\u2010phase conversion at the buried interface relative to the surface, creating kinetic mismatch that exacerbates moisture attack and defect accumulation. To address these kinetic and environmental constraints, we design a self\u2010segregating multifunctional molecule, 2\u2010[(3\u2010trifluoromethyl)phenyl]amino\u20103\u2010pyridinecarboxylic acid (NFA), which spontaneously enriches at the buried interface to synchronize dual\u2010interface crystallization while simultaneously passivating defects, optimizing energy\u2010level alignment, and constructing a hydrophobic barrier against moisture ingress. Consequently, this self\u2010segregated kinetic\u2013environmental regulation yields record ambient flexible photovoltaic performance with power\u2010conversion efficiencies of 24.84% (0.09\u00a0cm\n                    <jats:sup>2<\/jats:sup>\n                    , certified at 23.75%) and 21.46% on mini\u2010modules (13.8\u00a0cm\n                    <jats:sup>2<\/jats:sup>\n                    ). The optimized devices maintain 96.26% of their starting efficiency following 1000\u00a0h damp aging at 85\u00a0\u00b1\u00a05% RH. Our work establishes self\u2010segregated interfacial regulation as a rational route to address kinetic and environmental constraints in scalable flexible photovoltaics.\n                  <\/jats:p>","DOI":"10.1002\/adma.75474","type":"journal-article","created":{"date-parts":[[2026,10,22]],"date-time":"2026-10-22T10:59:20Z","timestamp":1792666760000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Self\u2010Segregated Buried\u2010Interface Regulation Resolves Kinetic\u2013Environmental Coupling for Ambient Flexible Perovskite Solar Cells"],"prefix":"10.1002","author":[{"given":"Chenxin","family":"Zhao","sequence":"first","affiliation":[{"name":"Key Laboratory of Applied Surface and Colloid Chemistry National Ministry of Education School of Materials Science and Engineering Shaanxi Normal University  Xi'an 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