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Adv. Mater., Aug 01 2026, | https://doi.org/10.1002/adma.74385 Play-Doh Inspired a Transformative, Shape-Adaptive iHEÄLS Enabling Post-Crosslinking Mechanical-Biological Modulation and Its Effectiveness in Musculoskeletal Repair

Niyou Wang ^{1 2}, Chao Liang ³, Soo A Kim ^{1 4}, Jessica Heline Lopes da Fonseca ¹⁵, María José Veana Hernandez ^{1 6}, Zahra Rezaei ¹, Alvaro Dario Martinez Blanco ^{1 7}, Nicole Joy Bassous ¹, Da Seul Kim ¹, Yejin Jo ^{1 4}, Tae Young Kim ⁴, Yipei Yang ¹ ⁸, Ziqi Huang ³, Siyuan Chen ³, Feiming Li ³, Marcos Akira dAvila ⁵, June-Seo Kim ⁹, Misun Kang ¹⁰, Jungmok Seo ⁴, Sang Jin Lee ³, Su Ryon Shin ¹

¹Division of Engineering in Medicine, Department of Medicine, Brigham and Women's Hospital, Harvard Medical School, Cambridge, Massachusetts, USA.
²Institute of Materials Research and Engineering (IMRE), Agency For Science, Technology and Research (A*STAR), Singapore, Singapore.
³Biofunctional Materials, Division of Applied Oral Sciences and Community Dental Care, Faculty of Dentistry, The University of Hong Kong, Sai Ying Pun, Hong Kong SAR, People's Republic of China.
⁴School of Electrical and Electronic Engineering, Yonsei University, Seoul, Republic of Korea.
⁵Department of Manufacturing and Materials Engineering, School of Mechanical Engineering, University of Campinas, Campinas, Brazil.
⁶Monterrey Institute of Technology, School of Engineering and Science, Heroica Puebla de Zaragoza, Puebla, Mexico.
⁷Monterrey Institute of Technology, School of Science and Engineering, Santiago de Querétaro, Querétaro, Mexico.
⁸Department of Orthopedic Surgery, The Second Affiliated Hospital of Guangzhou University of Chinese Medicine, Guangzhou, People's Republic of China.
⁹Division of Nanotechnology, Daegu Gyeongbuk Institute of Science & Technology (DGIST), Daegu, Republic of Korea.
¹⁰Department of Chemistry, Keimyung University, Daegu, Republic of Korea.

Correspondence: Sang Jin Lee, Su Ryon Shin
Niyou Wang, Chao Liang and Soo A Kim contributed equally to this work.

Abstract

Resorbable biomaterials are being developed as alternatives to traditional medical fillers for musculoskeletal repair. 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 iHEÄLS, a transformative, shape-adaptive biomaterial inspired by Play-Doh, composed of cellulose nanocrystal (CNC)-based triple-networks. The interactions among the triple-networks enable conformal defect filling, robust tissue adhesion, and shape stabilization through self-healing. Mechanical training after crosslinking reinforces the network through aligned polymer chains and uniformly oriented CNC. As a biodegradable extracellular matrix, iHEÄLS promotes cell migration and osteogenic differentiation by leveraging nanomaterial incorporation and post-crosslinking mechanical training to amplify bioactivity and mechanotransduction signaling. Additionally, iHEÄLS demonstrates enhanced hemostasis by quickly absorbing biofluids while maintaining malleability, facilitating effective mixing with autologous bone fragments, and promoting bone regeneration in a critical-sized calvarial defect model. Overall, iHEÄLS integrates post-crosslinking mechanical-biological modulability with user-friendly handling, providing a practical platform for musculoskeletal repair in emergencies.

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