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Here, we present a hierarchical bonding network strategy to realize stable adhesion under harsh underwater conditions. By engineering a cross\u2010linked polysiloxane backbone embedded with dense active interaction sites, including hydroxyl groups, benzene rings, cations, and hydrophobic moieties, we create synergistic multiscale interactions that amplify both cohesion and interfacial adhesion.\u00a0The optimized adhesive achieves a strong bonding strength of 12.2\u00a0MPa and an underwater adhesion of 3.4\u00a0MPa on steel substrates and retains stability in corrosive underwater environments (acidic, alkaline, and saline solutions) over extended periods. It further demonstrates exceptional thermal resilience, maintaining functionality across temperatures from \u2010196 to 150\u00a0\u00b0C.\u00a0Integrating quaternary ammonium cations with long\u2010chain alkanes endows the material with potent antibacterial activity (\u226599.9999% inhibition) and the highest antifungal grade. This work provides a new avenue for designing high\u2010performance multifunctional adhesives with strong adhesion, long\u2010term durability, extreme temperature resistance, and antimicrobial properties, offering broad potential for applications in demanding underwater environments.<\/jats:p>","DOI":"10.1002\/anie.202521651","type":"journal-article","created":{"date-parts":[[2026,1,6]],"date-time":"2026-01-06T07:17:30Z","timestamp":1767683850000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":23,"title":["Tailored Hierarchical Bonding Networks Derive Ultra\u2010Stable Underwater Adhesion in Harsh Environments"],"prefix":"10.1002","volume":"65","author":[{"given":"Shuang\u2010Mei","family":"He","sequence":"first","affiliation":[{"name":"State Key Laboratory of Advanced Polymer Materials Collaborative Innovation Center for Eco\u2010Friendly and Fire\u2010Safety Polymeric Materials (MoE) National Engineering Laboratory of 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