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However, most synthetic strategies failed to unite rapid healing, fatigue resistance, and environmental robustness, limited by their singular compositional\/structural designs. Here, we present a soft, tough, fatigue\u2010resistant, and self\u2010healable ionic elastomer (STFSI elastomer), which fuses skin\u2010like binary assembly and Bouligand helicoidal structure into a composite of thermoplastic polyurethane (TPU) fibers and a supramolecular ionic biopolymer. The interlocked binary assembly enables skin\u2010like softness, high stretchability, and strain\u2010adaptive stiffening through a matrix\u2010to\u2010scaffold stress transfer. The Bouligand structure contributes to superhigh fracture toughness (101.6\u2005kJ\u2009m<jats:sup>\u22122<\/jats:sup>) and fatigue resistance (4937\u2005J\u2009m<jats:sup>\u22122<\/jats:sup>) via mechanical toughening by interlayer slipping and twisted crack propagation path. Besides, the STFSI elastomer is self\u2010healable through a \u201cbridging\u201d method and environment\u2010tolerant (\u221220\u2009\u00b0C, strong acid\/alkali, saltwater). To demonstrate the versatile structural and sensing applications, we showcase a safety cushion with efficient damping and suppressed rebounding, and a robotic sensor with excellent fatigue crack tolerance and instant sensation recovery upon cutting\u2010off damage. Our presented synthetic strategy is generalizable to other fiber\u2010reinforced tough polymers for applications involving demanding mechanical\/environmental conditions.<\/jats:p>","DOI":"10.1002\/anie.202411418","type":"journal-article","created":{"date-parts":[[2024,7,10]],"date-time":"2024-07-10T09:54:26Z","timestamp":1720605266000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":25,"title":["A Soft, Fatigue\u2010free, and Self\u2010healable Ionic Elastomer via the Synergy of Skin\u2010like Assembly and Bouligand Structure"],"prefix":"10.1002","author":[{"given":"Xinyuan","family":"Jiang","sequence":"first","affiliation":[{"name":"State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of Ceramics Chinese Academy of Sciences  1295 Ding Xi Road Shanghai 200050 China"},{"name":"School of Chemistry and Materials Science Hangzhou Institute of Advanced Study University of Chinese Academy of Sciences  Hangzhou 310024 China"},{"name":"Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences  1 Sub-lane Xiangshan Beijing 100049 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yin","family":"Cheng","sequence":"additional","affiliation":[{"name":"State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of Ceramics Chinese Academy of Sciences  1295 Ding Xi Road Shanghai 200050 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Liangjing","family":"Shi","sequence":"additional","affiliation":[{"name":"State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of Ceramics Chinese Academy of Sciences  1295 Ding Xi Road Shanghai 200050 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jing","family":"Sun","sequence":"additional","affiliation":[{"name":"State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of Ceramics Chinese Academy of Sciences  1295 Ding Xi Road Shanghai 200050 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5097-2834","authenticated-orcid":false,"given":"Ranran","family":"Wang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of Ceramics Chinese Academy of Sciences  1295 Ding Xi Road Shanghai 200050 China"},{"name":"School of Chemistry and Materials Science Hangzhou Institute of Advanced Study University of Chinese Academy of Sciences  Hangzhou 310024 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