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Functional regeneration of the periodontium remains a major challenge due to the hierarchical soft\u2010hard tissue interface and complex spatiotemporal functional demands. In this study, a synchronously in situ co\u2010injectable, interlayer\u2010bonding, and wet\u2010adhesive bilayer hydrogel (Bio\u2010Fun bilayer) consisting of PCAC and PCMC layers is developed. An anti\u2010delamination interface is engineered via polymer chain topological entanglement and dynamic boronate ester and ionic networks, while precise complex viscosity matching enables synchronized microscale laminar co\u2010extrusion. Concurrently, the hydrogel maintains wet adhesion, especially to moist root and bone surfaces. Spatiotemporal biofunctionalization is achieved by loading microRNA\u201026a liposomes in the PCAC layer to activate Wnt\/\u03b2\u2010catenin signaling for osteogenesis, and covalently tethering a PDGF\u2010BB mimetic peptide within the PCMC layer to trigger PI3K\/Akt\u2010LOX signaling for fibroblast recruitment and functional collagen formation. In vivo, the Bio\u2010Fun bilayer hydrogel achieves integrated regeneration of alveolar bone and aligned periodontal ligament fibers, forming Sharpey's fiber\u2010like structures with firm bone\u2010ligament attachment. Meanwhile, the modular and injectable design might provide broad reference for the reconstruction of periodontal, osteochondral, and other soft\u2010hard tissue interfaces.<\/jats:p>","DOI":"10.1002\/adma.75042","type":"journal-article","created":{"date-parts":[[2026,9,22]],"date-time":"2026-09-22T07:07:31Z","timestamp":1790060851000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["A Tightly Interlayer Bonded, Synchronously In Situ Co\u2010Injectable, Wet\u2010Adhesive, Hierarchically Biofunctionalized Bilayer Hydrogel for Functional Attachment and Orderly Periodontal Regeneration"],"prefix":"10.1002","volume":"38","author":[{"ORCID":"https:\/\/orcid.org\/0009-0009-5964-6504","authenticated-orcid":false,"given":"Aijing","family":"Wang","sequence":"first","affiliation":[{"name":"Department of Cariology and Endodontology Peking University  Beijing P. R. 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