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Here, we show that the lactide\u2010to\u2010glycolide ratio of a PLGA\u2010PEG\u2010PLGA triblock copolymer directly controls interfacial interactions at the MXene surface and, through this mechanism, determines how well the encapsulated nanosheets resist oxidation over time. Combined computational and experimental analyses reveal that glycolide\u2010rich segments form dense hydrogen\u2010bonding networks at the MXene interface, providing effective surface protection despite accelerated bulk hydrolysis. This competing interplay defines a compositional window in which MXene stability and hydrogel degradability are simultaneously optimized, a balance we validate through combined DFT, molecular dynamics, and experimental characterization. Building on this design principle, we formulate a sprayable composite that gels in situ upon contact with tissue, conformally coating irregular wound surfaces without manual placement. The optimized hydrogel exhibits robust photothermal performance under physiological conditions and effectively suppresses tumor growth in a postoperative melanoma model. These findings highlight the importance of interfacial design in stabilizing oxidation\u2010sensitive nanomaterials within dynamic polymer systems and provide practical guidelines for developing durable MXene\u2010based biomedical platforms.\n                  <\/jats:p>","DOI":"10.1002\/smll.75631","type":"journal-article","created":{"date-parts":[[2026,9,9]],"date-time":"2026-09-09T15:07:25Z","timestamp":1788966445000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Sprayable MXene Hydrogels With Composition\u2010Driven Interfacial Stabilization and on\u2010Skin Gelation for Conformal Postsurgical Photothermal Therapy"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0007-1953-5223","authenticated-orcid":false,"given":"Taek","family":"Hwang","sequence":"first","affiliation":[{"name":"Biomaterials Research Center Korea Institute of Science and Technology (KIST)  Seoul Republic of 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Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4778-4629","authenticated-orcid":false,"given":"Youngmee","family":"Jung","sequence":"additional","affiliation":[{"name":"Biomaterials Research Center Korea Institute of Science and Technology (KIST)  Seoul Republic of Korea"},{"name":"School of Electrical and Electronic Engineering YU\u2010KIST Institute Yonsei University  Seoul Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5029-1593","authenticated-orcid":false,"given":"Bumjoon","family":"Seo","sequence":"additional","affiliation":[{"name":"Department of Chemical and Biomolecular Engineering Seoul National University of Science and Technology  Seoul Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5338-3856","authenticated-orcid":false,"given":"Seon 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