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Here, we report a molecularly engineered ionogel (VP\u2010IL) with a \u201crigid\u2013flexible combined skeleton,\u201d featuring bicontinuous phase separation via multiple supramolecular interactions. Created by copolymerizing rigid 1\u2010vinylimidazole (1\u2010VIM) and flexible 2\u2010phenoxyethyl acrylate (PhEA) with ionic liquid 1\u2010ethyl\u20103\u2010methylimidazolium bis(trifluoromethanesulfonyl)imide([EMIM][TFSI]) as dynamic crosslinker and phase\u2010separation driver, the VP\u2010IL ionogel exhibits a well\u2010defined bicontinuous phase separation orchestrated through strong cation\u2013\n                    <jats:italic>\u03c0<\/jats:italic>\n                    anchoring of [EMIM]\n                    <jats:sup>+<\/jats:sup>\n                    onto PhEA benzene rings. The synergistic interplay of this interaction with hydrogen bonds and\n                    <jats:italic>\u03c0<\/jats:italic>\n                    \u2013\n                    <jats:italic>\u03c0<\/jats:italic>\n                    stacking results in efficient energy dissipation and strain\u2010hardening in VP\u2010IL. Solid\u2010state NMR reveals the slow segmental motion activated by ionic liquids, thereby endowing the material with strong mechanical properties and charge transport capabilities. This dynamic network allows modulus switching over three orders of magnitude and rapid shape memory, supporting UV\u2010curable 3D printing. An intelligent TENG with a reconfigurable friction interface was developed by this material, whose output charge can be regulated on demand through micro\u2010patterning. This work offers a new material platform for the design of a new generation of adaptive soft robots and wearable self\u2010powered systems.\n                  <\/jats:p>","DOI":"10.1002\/smll.74157","type":"journal-article","created":{"date-parts":[[2026,6,18]],"date-time":"2026-06-18T10:10:19Z","timestamp":1781777419000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Thermally Reconfigurable Interfaces Engineered by Robust Ionogels for Intelligent TENG Signal Modulation"],"prefix":"10.1002","volume":"22","author":[{"given":"Jiawen","family":"Hou","sequence":"first","affiliation":[{"name":"Key Laboratory of Functional Polymer Materials of Ministry of Education Frontiers Science Center for New Organic Matter College of Chemistry Nankai University  Tianjin P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hanbing","family":"Ma","sequence":"additional","affiliation":[{"name":"Key Laboratory of Functional Polymer Materials of Ministry of Education Frontiers Science Center for New Organic Matter College of Chemistry Nankai University  Tianjin P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaoliang","family":"Wang","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering Nanjing University  Nanjing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Pingchuan","family":"Sun","sequence":"additional","affiliation":[{"name":"Key Laboratory of Functional Polymer Materials of Ministry of Education Frontiers Science Center for New Organic Matter College of Chemistry Nankai University  Tianjin P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fenfen","family":"Wang","sequence":"additional","affiliation":[{"name":"Key Laboratory of Functional Polymer Materials of Ministry of Education Frontiers Science Center for New Organic Matter College of Chemistry Nankai University  Tianjin P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,6,18]]},"reference":[{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202404451"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202212888"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202411172"},{"key":"e_1_2_7_5_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsami.3c05943"},{"key":"e_1_2_7_6_1","doi-asserted-by":"publisher","DOI":"10.1002\/smll.202304321"},{"key":"e_1_2_7_7_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202418941"},{"key":"e_1_2_7_8_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202207452"},{"key":"e_1_2_7_9_1","doi-asserted-by":"publisher","DOI":"10.1002\/smll.202403052"},{"key":"e_1_2_7_10_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202413901"},{"key":"e_1_2_7_11_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202416599"},{"key":"e_1_2_7_12_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202311214"},{"key":"e_1_2_7_13_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsami.2c11029"},{"key":"e_1_2_7_14_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-021-24382-4"},{"key":"e_1_2_7_15_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemmater.7b02402"},{"key":"e_1_2_7_16_1","doi-asserted-by":"publisher","DOI":"10.1002\/smll.202403252"},{"key":"e_1_2_7_17_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2023.144674"},{"key":"e_1_2_7_18_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202405965"},{"key":"e_1_2_7_19_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202414682"},{"key":"e_1_2_7_20_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jcis.2024.10.168"},{"key":"e_1_2_7_21_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsnano.4c02661"},{"key":"e_1_2_7_22_1","doi-asserted-by":"publisher","DOI":"10.1039\/D5TA01250C"},{"key":"e_1_2_7_23_1","doi-asserted-by":"publisher","DOI":"10.1007\/s40820-024-01387-4"},{"key":"e_1_2_7_24_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.nanoen.2021.106645"},{"key":"e_1_2_7_25_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsnano.4c12130"},{"key":"e_1_2_7_26_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-024-55245-3"},{"key":"e_1_2_7_27_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202214001"},{"key":"e_1_2_7_28_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsami.2c13294"},{"key":"e_1_2_7_29_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202500770"},{"key":"e_1_2_7_30_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41563-022-01195-4"},{"key":"e_1_2_7_31_1","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.adl2737"},{"key":"e_1_2_7_32_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202313781"},{"key":"e_1_2_7_33_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202211456"},{"key":"e_1_2_7_34_1","doi-asserted-by":"publisher","DOI":"10.1021\/ma300335p"},{"key":"e_1_2_7_35_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202408826"},{"key":"e_1_2_7_36_1","doi-asserted-by":"publisher","DOI":"10.1039\/D4TA01001A"},{"key":"e_1_2_7_37_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.4c01758"},{"key":"e_1_2_7_38_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2023.145177"},{"key":"e_1_2_7_39_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202405105"},{"key":"e_1_2_7_40_1","doi-asserted-by":"publisher","DOI":"10.1039\/D3MH01587D"},{"key":"e_1_2_7_41_1","doi-asserted-by":"publisher","DOI":"10.1002\/(SICI)1521-4044(19990801)50:8<271::AID-APOL271>3.0.CO;2-Y"},{"key":"e_1_2_7_42_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja992022v"},{"key":"e_1_2_7_43_1","volume-title":"Multidimensional 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