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This study provides direct structural and spectroscopic evidence of H\u2010bonded anionic wires in protic ionic liquids (PILs), which consist of triethylammonium cations and hydrogen dicarboxylate anions. The anionic wires were identified by X\u2010ray crystallography in the solid state, wherein the anions are linked by\n                    <jats:sup>\u2212<\/jats:sup>\n                    OH\u00b7\u00b7\u00b7O\n                    <jats:sup>\u2212<\/jats:sup>\n                    type H\u2010bonds. The H\u2010bonds within the anionic wire are significantly stronger than those between cation and anion despite repulsive Coulomb interaction in the first and attractive ones in the latter case. Analysis by nuclear magnetic resonance (NMR) and infrared (IR) spectroscopy suggests that the binding motifs of the solid structure are mainly preserved in the liquid state of the supercooled PILs. This conclusion is drawn from density functional theory (DFT) calculations of the same structural motifs as observed in the solid state. The calculated\n                    <jats:sup>1<\/jats:sup>\n                    H NMR chemical shifts and IR C\u2550O frequencies for these H\u2010bond structures correspond well with the measured spectroscopic signatures. The anionic chains remain intact even when gradually removing the counterions. Our findings highlight the fundamental role of hydrogen bonding for the unusual attractive interaction between ions of like charge.\n                  <\/jats:p>","DOI":"10.1002\/cphc.70581","type":"journal-article","created":{"date-parts":[[2026,9,30]],"date-time":"2026-09-30T05:35:32Z","timestamp":1790746532000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Structural and Spectroscopic Evidence of Hydrogen Bonded Anionic Wires in Protic Ionic Liquids"],"prefix":"10.1002","volume":"27","author":[{"ORCID":"https:\/\/orcid.org\/0009-0000-7860-4080","authenticated-orcid":false,"given":"Maham","family":"Azhar","sequence":"first","affiliation":[{"name":"Institut f\u00fcr Chemie Abteilung Physikalische Chemie Universit\u00e4t Rostock  Rostock Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lasse","family":"Hunger","sequence":"additional","affiliation":[{"name":"Institut f\u00fcr Chemie Abteilung Physikalische Chemie Universit\u00e4t Rostock  Rostock Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Loai","family":"Al\u2010Sheakh","sequence":"additional","affiliation":[{"name":"Institut f\u00fcr Chemie Abteilung Physikalische Chemie Universit\u00e4t Rostock  Rostock Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Andreas","family":"Appelhagen","sequence":"additional","affiliation":[{"name":"Institut f\u00fcr Chemie Abteilung Physikalische Chemie Universit\u00e4t Rostock  Rostock Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8631-1840","authenticated-orcid":false,"given":"Lennart","family":"Kruse","sequence":"additional","affiliation":[{"name":"Institut f\u00fcr Chemie Abteilung Physikalische Chemie Universit\u00e4t Rostock  Rostock Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8549-071X","authenticated-orcid":false,"given":"Ralf","family":"Ludwig","sequence":"additional","affiliation":[{"name":"Institut f\u00fcr Chemie Abteilung Physikalische Chemie Universit\u00e4t Rostock  Rostock Germany"},{"name":"Department Life, Light &amp; Matter Universit\u00e4t Rostock  Rostock Germany"},{"name":"Leibniz Institut f\u00fcr Katalyse an der Universit\u00e4t Rostock e.V.  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