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As a result, electrolytes are often treated as passive screening agents rather than active design parameters. Here, we show that electrolyte identity can deterministically regulate the mechanical state of soft interfaces through ion\u2010specific hydration effects. Using quaternized bottlebrush polymers on mica as a force\u2010resolved model system, we identify a two\u2010channel mechanism that separates polymer\u2010substrate interactions from interpolymer cohesion. Cation hydration controls access to surface binding sites: strongly hydrated Na\n                    <jats:sup>+<\/jats:sup>\n                    preserves polymer anchoring by remaining solvated near the surface, whereas weakly hydrated K\n                    <jats:sup>+<\/jats:sup>\n                    directly occupies lattice sites and suppresses adhesion. In parallel, anion valency activates a distinct cohesion pathway, where multivalent anions bridge polymer chains across the confined interface. Coupling between these pathways produces non\u2010additive behavior, enabling regimes in which substrate anchoring is suppressed while interpolymer bridging sustains adhesion. These findings establish electrolyte composition, not simply ionic strength, as a primary control parameter for interfacial mechanics, providing a framework for designing adaptive adhesion and hydration\u2010mediated interactions in aqueous environments.\n                  <\/jats:p>","DOI":"10.1002\/advs.78071","type":"journal-article","created":{"date-parts":[[2026,9,29]],"date-time":"2026-09-29T04:16:07Z","timestamp":1790655367000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Nonlinear Ion\u2010Specific Control of Underwater Adhesion by Bottlebrush Polymer Interfaces"],"prefix":"10.1002","author":[{"given":"Chang\u2010Sheng","family":"Wang","sequence":"first","affiliation":[{"name":"Faculty of Pharmacy Universit\u00e9 De Montr\u00e9al  Montr\u00e9al Qu\u00e9bec Canada"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hui","family":"Guo","sequence":"additional","affiliation":[{"name":"Faculty of 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