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However, polymers tend to exhibit strongly nonlinear conduction at high temperatures and under high electric fields, leading to a rapid increase in leakage current and typically limiting the stable operating temperature to around 250\u00b0C. Here, we report a coupled conformational and vibrational engineering strategy in polyimide (PI) dielectrics that weakens electronic coupling and suppresses specific molecular vibrations governing thermally assisted charge transport. This dual\u2010action design effectively delays the onset of high\u2010field nonlinear conduction and suppresses leakage current at extreme temperatures. Consequently, the resulting PI dielectric films achieve a maximum discharged energy density of 5.9 J cm\n                    <jats:sup>\u22123<\/jats:sup>\n                    at 300\u00b0C and maintain 2.8 J cm\n                    <jats:sup>\u22123<\/jats:sup>\n                    with 90% efficiency, while sustaining over 10\n                    <jats:sup>5<\/jats:sup>\n                    charge\u2013discharge cycles at 300\u00b0C, surpassing state\u2010of\u2010the\u2010art polymer dielectrics in operating temperature and cycling reliability. This strategy provides a fundamentally different route from conventional bandgap engineering approaches for high energy density polymer dielectrics operating at 300\u00b0C.\n                  <\/jats:p>","DOI":"10.1002\/adma.75078","type":"journal-article","created":{"date-parts":[[2026,9,23]],"date-time":"2026-09-23T13:22:40Z","timestamp":1790169760000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Record\u2010High Capacitive Energy Density in Polyimide Dielectrics\u00a0at 300\u00b0C via Conformational\u2013Vibrational Engineering"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0004-7087-5045","authenticated-orcid":false,"given":"Guanghu","family":"He","sequence":"first","affiliation":[{"name":"State Key Laboratory of Powder Metallurgy Central South University  Changsha Hunan Province P. R. 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