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Liquid crystal polymers (LCPs) and Cu are increasingly used owing to their thermal stability, chemical resistance, and electrical performance. However, weak interfacial adhesion limits reliable integration, particularly under mechanical or thermal stress. Conventional surface treatments, such as plasma etching and chemical modification, often require complex processing, cause surface damage, and lack scalability. Herein, a bifunctional adhesive with pyridine and silane terminals (PyAAc\u2010SiOH) is synthesized via Cu\u2010catalyzed azide\u2010alkyne cycloaddition (CuAAC) to address this challenge. Silanol groups enabled covalent bonding with hydroxylated LCP surfaces, and the pyridine moiety formed coordination bonding with Cu. Interfacial adhesion is evaluated using peel tests (ASTM D3359\u201097) and shear tests (ISO 4587), supported by morphological and spectroscopic analyses. At 1 wt% PyAAc\u2010SiOH, adhesion rating of 5B with 0.77% delamination was achieved, and optimal mechanical performance with lap shear strength of 3.84\u00a0MPa, ductility of 0.01, and toughness of 21.23\u00a0MJ\/m\n                    <jats:sup>3<\/jats:sup>\n                    . Fracture surface analysis indicates a concentration\u2010dependent transition from adhesive to cohesive and mixed failure modes, consistent with monolayer\u2010like interfacial behavior. Therefore, PyAAc\u2010SiOH enables efficient, damage\u2010free enhancement of Cu\u2010LCP adhesion through molecular\u2010level control, offering a scalable strategy for flexible substrates, packaging, and heterogeneous electronic integration.\n                  <\/jats:p>","DOI":"10.1002\/smtd.71025","type":"journal-article","created":{"date-parts":[[2026,9,7]],"date-time":"2026-09-07T07:27:11Z","timestamp":1788766031000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["A Click\u2010Derived Pyridine\u2010Silane Molecular Adhesive for Dual Covalent and Coordination Bonding at Metal\u2010Polymer Interfaces"],"prefix":"10.1002","volume":"10","author":[{"given":"Hyunlee","family":"Kim","sequence":"first","affiliation":[{"name":"Department of MetaBioHealth Sungkyunkwan University (SKKU)  Suwon Republic of 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