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This study correlates the emergence of interfacial\u2010water SERS signatures with electrolyte\u2010specific reconstruction of the local hydrogen\u2010bond environment within the electric double layer. In situ electrochemical SERS, constrained O\u2212H band deconvolution, quantum\u2010chemical cluster calculations, and molecular dynamics simulations are combined to compare roughened Ag electrodes in 1.0\u00a0M KCl and NaCl. The spectra reveal pronounced electrolyte\u2010 and potential\u2010dependent redistribution of the interfacial O\u2212H stretching response, accompanied by distinct ion\u2010hydration, hydrogen\u2010bond, and orientational structures in the simulations. Chloride\u2010associated interfacial species provide a plausible chemical\u2010enhancement contribution, whereas the more compact Na\n                    <jats:sup>+<\/jats:sup>\n                    hydration environment correlates with a larger retained high\u2010wavenumber O\u2212H contribution. The combined results support a mechanistic picture in which electrolyte\u2010induced hydration\u2010network reconstruction may modify intermolecular vibrational coupling and energy redistribution, thereby contributing to the SERS detectability of interfacial water.\n                  <\/jats:p>","DOI":"10.1002\/smtd.71139","type":"journal-article","created":{"date-parts":[[2026,10,21]],"date-time":"2026-10-21T11:32:13Z","timestamp":1792582333000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Surface\u2010Enhanced Raman Detection of Interfacial Water Enabled by Electrolyte\u2010Specific Reconstruction of Hydrogen\u2010Bond Network Defects in the Electric Double Layer"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0001-2021-7798","authenticated-orcid":false,"given":"Xing","family":"Zhong","sequence":"first","affiliation":[{"name":"Beijing Key Laboratory of Nanophotonics and Nanostructures Department of Physics Capital Normal University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wen\u2010Jing","family":"Bo","sequence":"additional","affiliation":[{"name":"Beijing Key Laboratory of Nanophotonics and Nanostructures Department of Physics Capital Normal University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jia\u2010Lei","family":"Yan","sequence":"additional","affiliation":[{"name":"Beijing Key Laboratory of Nanophotonics and Nanostructures Department of Physics Capital Normal University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xi","family":"Liang","sequence":"additional","affiliation":[{"name":"Beijing Key Laboratory of Nanophotonics and Nanostructures Department of Physics Capital Normal University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Li\u2010Sheng","family":"Zhang","sequence":"additional","affiliation":[{"name":"Beijing 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