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Herein, we report a multifunctional ionogel derived from a polymerizable deep eutectic solvent (PDES) composed of 1-ethyl-3-methylimidazolium bromide and acrylic acid (EmimBr\/AA), in which gallic acid (GA) is introduced as a multivalent hydrogen-bond donor and dynamic physical crosslinking hub, thereby eliminating the need for additional chemical crosslinkers. Benefiting from the synergistic effects of the PDES matrix and GA-mediated molecular-scale interactions, the resulting poly(EmimBr\/AA\/GA) ionogels exhibit a well-balanced set of properties, including a tensile strength of 0.84 MPa, an elongation at break of 1556%, high optical transparency (&amp;gt;92%), an ionic conductivity of 4.4 \u00d7 10\u20133 S m\u20131, and strong interfacial adhesion (54 kPa on copper). In addition, the reversible dynamic interactions endow the ionogels with intrinsic self-healing capability (91.2% healing efficiency after 4 h at 100 \u00b0C) and recyclability. As proof-of-concept applications, the ionogels were successfully integrated into skin-attachable strain sensors, a 4 \u00d7 4 tactile array, and a customized convolutional neural network-assisted smart glove, achieving classification accuracies of 98.5% for 10-class fine hand gestures and 99.08% for 5-class macroscopic body motions. This work offers a general strategy for constructing sustainable, crosslinker-free, high-performance ionogels for intelligent wearable electronics and advanced human\u2013machine interfaces.<\/jats:p>","DOI":"10.1021\/acsami.6c11640","type":"journal-article","created":{"date-parts":[[2026,9,9]],"date-time":"2026-09-09T19:02:25Z","timestamp":1788980545000},"page":"51601-51617","source":"Crossref","is-referenced-by-count":0,"title":["Gallic Acid-Crosslinked EmimBr\/AA Ionogels Derived from a Polymerizable Deep Eutectic Solvent toward Intelligent Human\u2013Machine Interfaces"],"prefix":"10.1021","volume":"18","author":[{"given":"Mengmeng","family":"Cao","sequence":"first","affiliation":[{"name":"Qilu University of Technology, Shandong Academy of Sciences , , ,","place":["Jinan, China, 250353"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3489-6920","authenticated-orcid":true,"given":"Nan","family":"Li","sequence":"additional","affiliation":[{"name":"Qilu University of Technology, Shandong Academy of Sciences , , ,","place":["Jinan, China, 250353"]},{"name":"Qufu Normal University , , ,","place":["Qufu, China, 273165"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xingxiang","family":"Ji","sequence":"additional","affiliation":[{"name":"Qilu University of Technology, Shandong Academy of Sciences , , ,","place":["Jinan, China, 250353"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8373-6117","authenticated-orcid":true,"given":"Wei","family":"Chen","sequence":"additional","affiliation":[{"name":"Qilu University of Technology, Shandong Academy of Sciences , , ,","place":["Jinan, China, 250353"]},{"name":"Qufu Normal University , , ,","place":["Qufu, China, 273165"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,9,9]]},"reference":[{"issue":"1","key":"2026092606072555900_cit1","doi-asserted-by":"publisher","first-page":"2029","DOI":"10.1021\/acsami.1c21325","article-title":"Ultrastretchable, Adhesive, Fast Self-Healable, and Three-Dimensional Printable Photoluminescent Ionic Skin Based on Hybrid Network Ionogels","volume":"14","author":"Hao","year":"2022","journal-title":"ACS Appl. 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