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Herein, six alkyl alkanolamide amphiphiles are designed, and their self\u2010assembly behavior in 1,2\u2010propanediol\/water cosolvent is investigated from 80 to \u221220\u00a0\u00b0C. The hydrocarbon chain length exerts a significant influence on self\u2010assembly behavior at both short\u2010range and long\u2010range scales. Amphiphiles with hydrocarbon chains shorter than C16 (i.e., the number of carbon atom is 16)\u00a0exhibit limited solubility and cannot form LLCs at low temperatures, while longer chains enhance cryo\u2010solubility and self\u2010assembly capabilities, contradicting conventional assumptions. Notably, amphiphiles with chains of C18 or longer require only 0.3\u00a0wt.% for LLCs formation. These LLCs exhibit intriguing temperature\u2010dependent phase transitions, including a liquid\u2010like lamellar phase, a tilted gel phase, and a distinct phase characterized by tighter alkyl chain packing. The hydrocarbon chain length directly governs the transition temperatures and further influences the long\u2010range orientational ordering of lamellar sheets. Additionally, the tightly\u2010packed configuration confers exceptional rheological properties, including ultra\u2010high viscosity, shear\u2010thinning behavior, and elasticity. These findings provide important insights for the design and engineering of high\u2010performance soft materials used in extreme environments.<\/jats:p>","DOI":"10.1002\/advs.202512502","type":"journal-article","created":{"date-parts":[[2025,9,15]],"date-time":"2025-09-15T19:29:39Z","timestamp":1757964579000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":5,"title":["Unlocking Cryogenic Self\u2010Assembly of Lyotropic Liquid Crystals: A Molecular Perspective From Short\u2010Range to Long\u2010Range Scales"],"prefix":"10.1002","volume":"12","author":[{"given":"Weiluo","family":"Guo","sequence":"first","affiliation":[{"name":"Polymer Research Institute State Key Laboratory of Advanced Polymer Materials Sichuan University  Chengdu 610065 P. R. 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