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Although numerous sunscreen materials have been developed, their performance remains limited by insufficient ultraviolet protection, low biosafety due to skin penetration of ultraviolet filters, poor skin adhesion, and a lack of therapeutic capacity for damaged tissues. Here a polyvinyl alcohol (PVA)\u2010based bilayer hydrogel fabricated by in situ assembly is reported. During gelation, interpenetration and cross\u2010linking of PVA chains at the interface fuse the two layers into an integrated structure. The resulting hydrogel exhibits exceptional ultraviolet absorption (SPF 1997.6 PA++++)\u2014twentyfold greater than previously reported values\u2014robust skin adhesion (317 J m\n                    <jats:sup>\u22122<\/jats:sup>\n                    ), photothermally controlled transdermal drug delivery (over 12\u00a0h), and excellent biocompatibility. The top layer employs template\u2010directed enzymatic polymerization of dopamine to produce polydopamine (PDA) nanoparticles that are firmly anchored within the PVA network. Extensive hydrogen bonding between PVA and PDA reduces the bandgap of PDA and enhances electron delocalization, markedly enhancing ultraviolet absorption. The bottom layer incorporates polysaccharides that confer robust skin adhesion and regulate drug release. This layered design enables the integration of skin protection and therapy, providing a generalizable approach for engineering complex soft materials.\n                  <\/jats:p>","DOI":"10.1002\/smll.202510083","type":"journal-article","created":{"date-parts":[[2025,12,2]],"date-time":"2025-12-02T09:41:13Z","timestamp":1764668473000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["In Situ Assembly of Bilayer Hydrogels by Templated Enzymatic Polymerization for Ultrahigh UV Absorption and Photothermal Transdermal Therapy"],"prefix":"10.1002","volume":"22","author":[{"given":"Bingqian","family":"Jiao","sequence":"first","affiliation":[{"name":"School of Chemical Science and Engineering Tongji University  Shanghai 200092 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yinghui","family":"Shang","sequence":"additional","affiliation":[{"name":"School of Chemical Science and Engineering Tongji University  Shanghai 200092 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dingze","family":"Zhou","sequence":"additional","affiliation":[{"name":"School of Chemical Science and Engineering Tongji University  Shanghai 200092 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xia","family":"Wang","sequence":"additional","affiliation":[{"name":"School of Chemical Science and Engineering Tongji University  Shanghai 200092 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4026-3337","authenticated-orcid":false,"given":"Qigang","family":"Wang","sequence":"additional","affiliation":[{"name":"School of Chemical Science and Engineering Tongji University  Shanghai 200092 P. R. China"},{"name":"Shanghai Key Laboratory of Anesthesiology and Brain Functional Modulation, Clinical Research Center for Anesthesiology and Perioperative Medicine, Translational Research Institute of Brain and Brain\u2010Like Intelligence, Shanghai Fourth People's Hospital, School of Medicine Tongji University  Shanghai 200434 P. R. China"},{"name":"National Key Laboratory of Autonomous Intelligent Unmanned Systems Tongji University  Shanghai 200092 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,12,2]]},"reference":[{"key":"e_1_2_8_1_1","doi-asserted-by":"publisher","DOI":"10.1038\/nrmicro.2017.157"},{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41577-018-0084-5"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1038\/nri3646"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1038\/nature13111"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1111\/jocd.14033"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1038\/nchembio.1548"},{"key":"e_1_2_8_7_1","doi-asserted-by":"publisher","DOI":"10.1007\/s00011-022-01598-8"},{"key":"e_1_2_8_8_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.aaa6806"},{"key":"e_1_2_8_9_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41586-020-2785-8"},{"key":"e_1_2_8_10_1","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.abd7703"},{"key":"e_1_2_8_11_1","doi-asserted-by":"publisher","DOI":"10.1038\/nnano.2010.25"},{"key":"e_1_2_8_12_1","doi-asserted-by":"publisher","DOI":"10.1111\/jocd.14004"},{"key":"e_1_2_8_13_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsabm.0c00280"},{"key":"e_1_2_8_14_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.scitotenv.2020.142486"},{"key":"e_1_2_8_15_1","doi-asserted-by":"publisher","DOI":"10.3390\/cosmetics6040064"},{"key":"e_1_2_8_16_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41578-022-00483-4"},{"key":"e_1_2_8_17_1","doi-asserted-by":"publisher","DOI":"10.1021\/cr000108x"},{"key":"e_1_2_8_18_1","doi-asserted-by":"publisher","DOI":"10.1038\/natrevmats.2016.71"},{"key":"e_1_2_8_19_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.aaf3627"},{"key":"e_1_2_8_20_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.1214804"},{"key":"e_1_2_8_21_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202401035"},{"key":"e_1_2_8_22_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.201802127"},{"key":"e_1_2_8_23_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202011176"},{"key":"e_1_2_8_24_1","doi-asserted-by":"publisher","DOI":"10.1007\/s40820-023-01084-8"},{"key":"e_1_2_8_25_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41551-025-01374-z"},{"key":"e_1_2_8_26_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202007829"},{"key":"e_1_2_8_27_1","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.aau8528"},{"key":"e_1_2_8_28_1","first-page":"127","volume":"40","author":"Diffey B.","year":"1989","journal-title":"J. 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