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At temperatures relevant to wide\u2010bandgap semiconductor electronics (&gt;150\u00b0C), heat\u2010resistant polymer films must be heavily derated to avoid premature aging due to intensive hot\u2010carrier injection. Inspired by multilayered barrier structures in nature, we developed a scalable roll\u2010to\u2010roll self\u2010assembled organic\u2010inorganic nanolaminate coating that significantly enhances the high\u2010temperature dielectric performance of polymer films. The nanolaminate architecture introduces dual confinement mechanisms: nanoconfinement of the polymer binder suppresses chain motion and enhances thermal stability, while anisotropic carrier relaxation within two\u2010dimensional nanoclay nanosheets impedes through\u2010plane hot\u2010carrier transport. Together, these effects synergistically establish an interface\u2010rectification mechanism that promotes in\u2010plane energy dissipation and suppresses carrier injection at electrode\u2010polymer interfaces. At 150\u00b0C, the coating significantly reduces the pre\u2010breakdown conduction current of polyetherimide (PEI), increases the breakdown strength from 450 to 501 MV\/m, and improves the discharged energy density at 95% efficiency by 105%. Furthermore, roll\u2010to\u2010roll\u2010coated PEI capacitors exhibit a 45\u2010fold lifetime enhancement at 150\u00b0C and 180 MV\/m\u2014a design field previously sustained only by BOPP below 60\u00b0C. This work provides a scalable and technology\u2010ready strategy for high\u2010temperature, high\u2010density polymer capacitive energy storage.<\/jats:p>","DOI":"10.1002\/advs.78275","type":"journal-article","created":{"date-parts":[[2026,10,15]],"date-time":"2026-10-15T03:43:46Z","timestamp":1792035826000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Interface Rectification via Roll\u2010to\u2010Roll Dual\u2010Confinement Nanocoatings for High\u2010Temperature Polymer Capacitors"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-1083-3260","authenticated-orcid":false,"given":"Ning","family":"Guo","sequence":"first","affiliation":[{"name":"Electrical Insulation Research Center Institute of Materials Science University of Connecticut  Storrs Connecticut USA"},{"name":"Department of Electrical and Computer Engineering University of Connecticut  Storrs Connecticut USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Marina","family":"Dabaghian","sequence":"additional","affiliation":[{"name":"Department of Chemical and Biomolecular Engineering University of Connecticut  Storrs Connecticut USA"},{"name":"Polymer Program Institute of Materials Science University of Connecticut  Storrs Connecticut USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jierui","family":"Zhou","sequence":"additional","affiliation":[{"name":"GE Vernova Advanced Research Center  Niskayuna New York USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Josh N.","family":"Bodin","sequence":"additional","affiliation":[{"name":"Department of Chemical and Biomolecular Engineering University of Connecticut  Storrs Connecticut USA"},{"name":"Polymer Program Institute of Materials Science University of Connecticut  Storrs Connecticut USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0005-9212-5218","authenticated-orcid":false,"given":"Chong","family":"Xiang","sequence":"additional","affiliation":[{"name":"Department of Chemical and Biomolecular Engineering University of Connecticut  Storrs Connecticut USA"},{"name":"Polymer Program Institute of Materials Science University of Connecticut  Storrs Connecticut USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fei","family":"Wang","sequence":"additional","affiliation":[{"name":"Department of Materials Science &amp; 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