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However, current materials fail to provide stable wound sealing and tissue regeneration due to inadequate conformal adaptability to irregular defects, weak adhesion in wet environments, and insufficient mechanical robustness balanced with biodegradability. Here, we present iHE\u00c4LS, a transformative, shape\u2010adaptive biomaterial inspired by Play\u2010Doh, composed of cellulose nanocrystal (CNC)\u2010based triple\u2010networks. The interactions among the triple\u2010networks enable conformal defect filling, robust tissue adhesion, and shape stabilization through self\u2010healing. Mechanical training after crosslinking reinforces the network through aligned polymer chains and uniformly oriented CNC. As a biodegradable extracellular matrix, iHE\u00c4LS promotes cell migration and osteogenic differentiation by leveraging nanomaterial incorporation and post\u2010crosslinking mechanical training to amplify bioactivity and mechanotransduction signaling. Additionally, iHE\u00c4LS demonstrates enhanced hemostasis by quickly absorbing biofluids while maintaining malleability, facilitating effective mixing with autologous bone fragments, and promoting bone regeneration in a critical\u2010sized calvarial defect model. Overall, iHE\u00c4LS integrates post\u2010crosslinking mechanical\u2010biological modulability with user\u2010friendly handling, providing a practical platform for musculoskeletal repair in emergencies.<\/jats:p>","DOI":"10.1002\/adma.74385","type":"journal-article","created":{"date-parts":[[2026,8,1]],"date-time":"2026-08-01T16:39:52Z","timestamp":1785602392000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Play\u2010Doh Inspired a Transformative, Shape\u2010Adaptive iHE\u00c4LS Enabling Post\u2010Crosslinking Mechanical\u2010Biological Modulation and Its Effectiveness in Musculoskeletal Repair"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-3311-6793","authenticated-orcid":false,"given":"Niyou","family":"Wang","sequence":"first","affiliation":[{"name":"Division of Engineering in Medicine Department of Medicine Brigham and Women's Hospital Harvard Medical School  Cambridge Massachusetts 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