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While mussel\u2010inspired catechol\u2010based adhesives hold promise, current designs often neglect the role of molecular diversity in tuning cohesion\u2013adhesion dynamics. Inspired by the hierarchical branching of trees, where branch length and position determine fruit composition, we developed a structurally tunable bioadhesive platform by grafting five DOPA\u2010derived catechol derivatives\u2014varying in side\u2010chain length and substituents\u2014onto polyvinyl alcohol (PVA) via esterification. Computational, spectroscopic, structural, and mechanical analyses revealed that side\u2010chain length and substituents critically modulate the adhesive and cohesive properties of the hydrogels. Among these, the PVA\u2010CA system exhibited superior cohesion and adhesion across diverse substrates, attributed to the extended side chain and conjugated double bond of caffeic acid (CA) that enhance intramolecular packing and interfacial interactions. Ex vivo adhesion on porcine\/canine cardiac, pulmonary, and intestinal tissues, along with in vivo studies in hepatic defect and skin wound models, confirmed strong adhesion, biocompatibility, and improved tissue regeneration of PVA\u2010CA hydrogel. This work establishes a programmable molecular design strategy for next\u2010generation wet\u2010tissue adhesives with broad biomedical potential.<\/jats:p>","DOI":"10.1002\/advs.202521272","type":"journal-article","created":{"date-parts":[[2026,1,7]],"date-time":"2026-01-07T14:37:11Z","timestamp":1767796631000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":11,"title":["Catechol Derivative\u2010Based Bioadhesives: Molecular Design for Precision Medical Adhesion"],"prefix":"10.1002","volume":"13","author":[{"given":"Xueyu","family":"Wang","sequence":"first","affiliation":[{"name":"Chongqing Key Laboratory of Oral Diseases Chongqing Municipal Key Laboratory of Oral Biomedical Engineering of Higher Education Chongqing Municipal Health Commission Key Laboratory of Oral \u00a0Biomedical \u00a0Engineering The Affiliated Stomatological Hospital of Chongqing Medical University Chongqing 401147 P. R. 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