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Although significant progress has been made in device performance, meeting commercial demands remains a challenge in the aspects of long\u2010term stability and high external quantum efficiency (EQE). Here, an in situ crystallization regulation strategy is developed for optimizing red perovskite films through ingenious vapor design. Mixed vapor containing dimethyl sulfoxide and carbon disulfide (CS\n                    <jats:sub>2<\/jats:sub>\n                    ) is incorporated to conventional annealing, which contributes to thermodynamics dominated perovskite crystallization for well\u2010aligned cascade phase arrangement. Additionally, the perovskite surface defect density is minimized by the CS\n                    <jats:sub>2<\/jats:sub>\n                    molecule adsorption. Consequently, the target perovskite films exhibit smooth exciton energy transfer, reduced defect density, and blocked ion migration pathways. Leveraging these advantages, spectrally stable red PeLEDs are obtained featuring emission at 668, 656, and 648\u00a0nm, which yield record peak EQEs of 30.08%, 32.14%, and 29.04%, along with prolonged half\u2010lifetimes of 47.7, 60.0, and 43.7\u00a0h at the initial luminances of 140, 250, and 270\u00a0cd m\n                    <jats:sup>\u22122<\/jats:sup>\n                    , respectively. This work provides a universal strategy for optimizing perovskite crystallization and represents a significant stride toward the commercialization of red PeLEDs.\n                  <\/jats:p>","DOI":"10.1002\/adma.202410255","type":"journal-article","created":{"date-parts":[[2024,9,3]],"date-time":"2024-09-03T02:22:23Z","timestamp":1725330143000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":206,"title":["Efficient and Stable Red Perovskite Light\u2010Emitting Diodes via Thermodynamic Crystallization Control"],"prefix":"10.1002","volume":"36","author":[{"given":"Shi\u2010Chi","family":"Feng","sequence":"first","affiliation":[{"name":"Institute of Functional Nano and Soft Materials (FUNSOM) Jiangsu Key Laboratory for Carbon\u2010Based Functional Materials and Devices Soochow University  Suzhou Jiangsu 215123 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Facility Zhangjiang Laboratory Chinese Academy of Sciences  Shanghai 200241 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kai","family":"Zhang","sequence":"additional","affiliation":[{"name":"Macao Institute of Materials Science and Engineering (MIMSE) Faculty of Innovation Engineering Macau University of Science and Technology  Taipa Macao 999078 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bing\u2010Feng","family":"Wang","sequence":"additional","affiliation":[{"name":"School of Physics and Electronic Science East China Normal University  Shanghai 200062 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Long\u2010Xue","family":"Cao","sequence":"additional","affiliation":[{"name":"Institute of Functional Nano and Soft Materials (FUNSOM) Jiangsu Key Laboratory for Carbon\u2010Based Functional Materials and Devices Soochow University  Suzhou Jiangsu 215123 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