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Here, this trilemma is overcome via a dipole\u2010regulation strategy, confining polar methyl\u2010sulfonyl groups within a rigid semi\u2010aromatic polyimide framework using flexible methylene linkers. This dipole confinement domain structure of sulfonyl\u2010methylene\u2010benzene decouples dipolar response from charge transport: the flexible linkers enable polarization, while the rigid semi\u2010aromatic framework localizes charges and suppresses conduction. It results in a stable dipole network, yielding a material (STPCB\u2010PI) with a wide bandgap (4.38\u00a0eV) and a record\n                    <jats:italic>T<\/jats:italic>\n                    <jats:sub>g<\/jats:sub>\n                    (&gt;400\u00b0C). It achieves a high\n                    <jats:italic>\u03b5<\/jats:italic>\n                    <jats:sub>r<\/jats:sub>\n                    of 5.8, a modulus of 6.7\u00a0GPa, and exceptional energy storage, delivering 12.00\u00a0J\u00a0cm\n                    <jats:sup>\u22123<\/jats:sup>\n                    with 97% efficiency at 25\u00b0C, 9.98\u00a0J\u00a0cm\n                    <jats:sup>\u22123<\/jats:sup>\n                    with 94% efficiency at 150\u00b0C, and retaining 8.62\u00a0J\u00a0cm\n                    <jats:sup>\u22123<\/jats:sup>\n                    with 90% efficiency at 200\u00b0C, 293% improvement over the state\u2010of\u2010the\u2010art commercial polyetherimide. Even at 250\u00b0C, it maintains 4.24\u00a0J\u00a0cm\n                    <jats:sup>\u22123<\/jats:sup>\n                    with 93% efficiency. It also exhibits excellent self\u2010healing and cyclic endurance. This work sets a new performance benchmark and establishes a generalizable design paradigm that reconciles the intrinsic conflict between polarization and insulation in high\u2010temperature dielectric polymers.\n                  <\/jats:p>","DOI":"10.1002\/adma.74073","type":"journal-article","created":{"date-parts":[[2026,7,15]],"date-time":"2026-07-15T10:34:58Z","timestamp":1784111698000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["A Dipole\u2010Confined Charge Transport Paradigm for Ultrahigh\u2010Temperature Dielectric Polymers"],"prefix":"10.1002","volume":"38","author":[{"ORCID":"https:\/\/orcid.org\/0009-0002-3799-4996","authenticated-orcid":false,"given":"Zunchu","family":"Liu","sequence":"first","affiliation":[{"name":"PCFM Lab, GD HPPC Lab, Guangdong Engineering Technology Research Centre For High\u2010Performance Organic and Polymer Photoelectric Functional Films, GBRCE For Functional Molecular Engineering, State Key Laboratory of Optoelectronic Materials and Technologies, School of Chemistry, IGCME Sun Yat\u2010Sen University  Guangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kaijin","family":"Chen","sequence":"additional","affiliation":[{"name":"PCFM Lab, GD HPPC Lab, Guangdong Engineering Technology Research Centre For High\u2010Performance Organic and Polymer Photoelectric Functional Films, GBRCE For Functional Molecular Engineering, State Key Laboratory of Optoelectronic Materials and Technologies, School of Chemistry, IGCME Sun Yat\u2010Sen University  Guangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5106-1175","authenticated-orcid":false,"given":"Xueyi","family":"Yu","sequence":"additional","affiliation":[{"name":"PCFM Lab, GD HPPC Lab, Guangdong Engineering Technology Research Centre For High\u2010Performance Organic and Polymer Photoelectric Functional Films, GBRCE For 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