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Here, an efficient and scalable artificial molting strategy, based on self\u2010assembly of cellulose nanocrystals and subsequent mineralization of amorphous calcium carbonate, is developed to produce biomimetic materials with an exceptional combination of mechanical and photonic properties that are usually mutually exclusive in synthetic materials. These biomimetic composites exhibit tunable mechanics from \u201cstrong and flexible\u201d, which\u00a0exceeds the benchmark of natural chiral materials, to \u201cstiff and hard\u201d, which is comparable to natural and synthetic counterparts. Especially, the biomimetic composites possess ultrahigh stiffness of 2\u00a0GPa in their fully water\u2010swollen state\u2014a value well beyond hydrated crab exoskeleton, cartilage, tendon, and stiffest synthetic hydrogels, combined with exceptional strength and resilience. Additionally, these composites are distinguished by the tunable chiral structural color and water\u2010triggered switchable photonics that are absent in most artificial mineralized materials, as well as unique hydroplastic properties. This study opens the door for a scalable synthesis of resilient biophotonic structural materials in practical bulk form.<\/jats:p>","DOI":"10.1002\/adma.202206509","type":"journal-article","created":{"date-parts":[[2022,10,8]],"date-time":"2022-10-08T04:50:05Z","timestamp":1665204605000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":69,"title":["Bioinspired Chiral Template Guided Mineralization for Biophotonic Structural Materials"],"prefix":"10.1002","volume":"34","author":[{"given":"Rui","family":"Xiong","sequence":"first","affiliation":[{"name":"State Key Laboratory of Polymer Materials Engineering Polymer Research Institute of Sichuan University  Chengdu 610065 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wanlin","family":"Wu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Polymer Materials Engineering Polymer Research Institute of Sichuan University  Chengdu 610065 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