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Herein, a multifunctional hydrophobic ionogel is developed through in situ UV-initiated copolymerization of tert-butyl acrylate (tBA), 2-(dimethylamino)ethyl methacrylate (DMAEMA), and di(ethylene glycol) ethyl ether acrylate (DEEA) in the hydrophobic ionic liquid 1-ethyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide ([EMIm][TFSI]). Strong ion-dipole interactions and hydrogen bonding between DMAEMA segments and TFSI\u2013 anions establish a dynamic supramolecular network, endowing the ionogel with ultrafast self-healing, excellent environmental tolerance, and robust adhesion in both air and underwater environments. The optimized ionogel exhibits high transparency (&amp;gt;96%), stable ionic conductivity (1.17 mS cm\u20131), excellent flexibility, and high hydrophobicity with a water contact angle of 116\u00b0. Notably, the ionogel achieves rapid self-healing with efficiencies of 98% within 30 s in air and 95% within 5 min underwater without external stimulation, while its sensing and conductive performances are almost fully restored after repeated damage-healing cycles. Benefiting from stable ion transport channels and a robust dynamic network, the ionogel-based sensor displays high sensitivity, rapid response, excellent cycling durability, and reliable underwater sensing capability. As a proof of concept, the ionogel sensor is further employed for underwater Morse-code communication and can be integrated with an Arduino-based Internet of Things (IoT) platform to demonstrate a wearable emergency alarm system operable in both air and underwater environments. This work provides a versatile strategy for developing next-generation self-healing ionogels for wearable electronics, underwater communication, intelligent sensing, and emergency rescue systems.<\/jats:p>","DOI":"10.1021\/acsami.6c11185","type":"journal-article","created":{"date-parts":[[2026,10,5]],"date-time":"2026-10-05T18:01:30Z","timestamp":1791223290000},"page":"55205-55220","source":"Crossref","is-referenced-by-count":0,"title":["Dynamic Supramolecular Hydrophobic Ionogels with Ultrafast Self-Healing for Reliable Underwater Electronics"],"prefix":"10.1021","volume":"18","author":[{"given":"Yunbo","family":"Mo","sequence":"first","affiliation":[{"name":"Sichuan University , , ,","place":["Chengdu, P. R. China, 610065"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7493-9377","authenticated-orcid":true,"given":"Yafang","family":"Wang","sequence":"additional","affiliation":[{"name":"Sichuan University , , ,","place":["Chengdu, P. 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