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However, large\u2010area high\u2010quality organic single crystals are rarely obtained on the elastomer substrates commonly used in flexible electronics. Herein, inspired by soil salinization, we developed a segregation strategy to in situ grow large\u2010area organic single crystals on elastomer substrates via a simple air\u2013water interface drop\u2010casting method. Solvent\u2010evaporation\u2010driven phase separation in organic semiconductor\u2010elastomer blends promotes molecular migration, leading to a precipitation behaviour that enables the fabrication of centimetre\u2010scale organic single\u2010crystal nanosheet film directly on elastomer surfaces. Planar APS devices based on a mode molecule, 2,7\u2010dioctyl[1]benzothieno[3,2\u2010b][1]benzothiophene (C8\u2010BTBT), demonstrate exceptional synaptic functionality, including 171% paired\u2010pulse facilitation (PPF) and ultralow power consumption of 0.15 fJ per synaptic event. Leveraging a synergistic stress\u2010dispersion mechanism involving nanosheet sliding and elastic substrate deformation, these devices retain synaptic performance under 15% tensile strain and after 60 days of ambient storage without encapsulation. The results shed light on the large\u2010area fabrication of organic single crystals on elastomer toward high\u2010performance flexible neuromorphic electronics.<\/jats:p>","DOI":"10.1002\/smll.75292","type":"journal-article","created":{"date-parts":[[2026,8,18]],"date-time":"2026-08-18T09:46:44Z","timestamp":1787046404000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Elastomer\u2010Assisted Segregation Growth of Large\u2010Scale Stretchable Organic Crystalline Films for Flexible Photosynapses"],"prefix":"10.1002","volume":"22","author":[{"given":"Shao\u2010Hua","family":"Wang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Flexible Electronics (LoFE) Institute of Advanced Materials (IAM) School of Flexible Electronics (Future Technologies) Nanjing Tech University (Nanjing Tech)  Nanjing 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