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However, current ionogels still struggle to achieve a combination of mechanical robustness and tissue\u2010like anisotropy, hindering their application in next\u2010generation intelligent biomimetic materials. Inspired by the anisotropic structure of tendons, we have embedded parallel\u2010aligned rigid fiber bundles within a flexible ionogel to establish a tight interfacial bonding through supramolecular interlocking. This design enables the dispersion of stress and dissipation of energy through shear deformation of the ionogel in the parallel direction while maintaining high flexibility and stretchability in the perpendicular direction. Thus, tough anisotropic composite ionogels (ACIGs) can be constructed, which exhibit high strength, high modulus, as well as pronounced strength and stiffness anisotropies. The mechanical properties and anisotropies far surpass those of current anisotropic gel materials. Additionally, ACIG demonstrates excellent crack resistance, a wide operational temperature range, and high adhesiveness. It can serve as a biomimetic ligament to secure artificial joints, maintaining stability even after 10\u00a0000 bending cycles. Moreover, the conductive properties enable ACIG to function as a sensor for detecting joint movements and transmitting information, holding significant application potential in fields such as intelligent equipment and wearable devices.<\/jats:p>","DOI":"10.1002\/adma.202511903","type":"journal-article","created":{"date-parts":[[2026,1,19]],"date-time":"2026-01-19T13:16:39Z","timestamp":1768828599000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":21,"title":["Supramolecular Interlocking Produces Mechanically Anisotropic, Robust, and Tough Biomimetic Ionogels"],"prefix":"10.1002","volume":"38","author":[{"given":"Jiahao","family":"Kang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Green and Efficient Development of Phosphorus Resources Key Laboratory of Advanced Materials Technologies International (Hong Kong Macao and Taiwan) Joint Laboratory on Advanced Materials Technologies College of Materials 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