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However, HHSMs have weak mechanical properties that limit their practical applications. Inspired by the mechanical training\u2010driven structural remodeling strategy (MTDSRS) in biological tissues, herein, engineered MTDSRS is developed for self\u2010reinforcement of HHSMs to improve their inherent mechanical properties and broaden potential utility. The MTDSRS consists of repetitive mechanical training and solvent\u2010induced conformation transitions. Solvent\u2010induced conformation transition enables the formation of \u03b2\u2010sheet physical crosslinks among the proteins, while the repetitive mechanical loading allows the rearrangement of physically crosslinked proteins along the loading direction. Such synergistic effects produce strong and stiff mechanically trained\u2010HHSMs (MT\u2010HHSMs). The fracture strength and Young's modulus of the resultant MT\u2010HHSMs (water content of 43 <jats:bold>\u00b1<\/jats:bold> 4%)\u00a0reach 4.7 <jats:bold>\u00b1<\/jats:bold> 0.9\u00a0and 21.3 <jats:bold>\u00b1<\/jats:bold> 2.1\u00a0MPa,\u00a0respectively, which are 8\u2010fold stronger and 13\u2010fold stiffer than those of the as\u2010prepared HHSMs, as well as superior to most previously reported HHSMs with comparable water content. In addition, the animal silk\u2010like highly oriented molecular crosslinking network structure also provides MT\u2010HHSMs with fascinating physical and functional features, such as stress\u2010birefringence responsibility, humidity\u2010induced actuation, and repeatable self\u2010folding deformation.<\/jats:p>","DOI":"10.1002\/smll.202102660","type":"journal-article","created":{"date-parts":[[2021,7,20]],"date-time":"2021-07-20T05:45:46Z","timestamp":1626759946000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":24,"title":["Mechanical Training\u2010Driven Structural Remodeling: A Rational Route for Outstanding Highly Hydrated Silk Materials"],"prefix":"10.1002","volume":"17","author":[{"given":"Ting","family":"Shu","sequence":"first","affiliation":[{"name":"School of Physical Science and Technology ShanghaiTech University  393 Middle Huaxia Road Shanghai 201210 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