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Using complementary neutron spin echo spectroscopy and nuclear magnetic resonance diffusometry, we probe local and long-range dynamics of three protic ionic liquids over time scales from 10\u201312 to 10\u20133 seconds. We identify a fast relaxation with closely corresponding self and collective time scales, indicating cooperative rearrangement of the surrounding molecular network. Its characteristic time scale correlates with bulk viscosity, while its temperature dependence reveals distinct Arrhenius activation energies depending on whether extended networks are dominated by hydrogen bonding or electrostatic interactions. These results link cooperative network relaxation to macroscopic viscosity and show how molecular structure can tune the energetic cost of structural relaxation through network connectivity.<\/jats:p>","DOI":"10.1021\/acs.jpclett.6c02640","type":"journal-article","created":{"date-parts":[[2026,10,1]],"date-time":"2026-10-01T22:01:24Z","timestamp":1790892084000},"page":"11778-11783","source":"Crossref","is-referenced-by-count":0,"title":["Cooperative\nRelaxation Governs the Viscosity of Ionic\nLiquids"],"prefix":"10.1021","volume":"17","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-1840-3866","authenticated-orcid":true,"given":"Shurui","family":"Miao","sequence":"first","affiliation":[{"name":"The University of Sydney , , , ,","place":["Sydney, NSW, Australia, 2006"]},{"name":"University of Oxford , , ,","place":["Oxford, United Kingdom, OX13QZ"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bela","family":"Farago","sequence":"additional","affiliation":[{"name":"Institut Max von Laue-Paul Langevin (ILL) , 71 avenue des Martyrs, CS 20156, Cedex 9 , , ,","place":["Grenoble, France, F-38042"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7178-6467","authenticated-orcid":true,"given":"Ingo","family":"Hoffmann","sequence":"additional","affiliation":[{"name":"Institut Max von Laue-Paul Langevin (ILL) , 71 avenue des Martyrs, CS 20156, Cedex 9 , , ,","place":["Grenoble, France, F-38042"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8781-7854","authenticated-orcid":true,"given":"Rob","family":"Atkin","sequence":"additional","affiliation":[{"name":"The University of Western Australia , , , ,","place":["Perth, WA, Australia, 6009"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7262-7115","authenticated-orcid":true,"given":"Michael","family":"Gradzielski","sequence":"additional","affiliation":[{"name":"Technische Universita\u0308t Berlin , , Stra\u00dfe des 17. 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