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Interface engineering has emerged as a powerful strategy to introduce charge traps or construct interfacial barriers, thereby regulating carrier dynamics and enhancing energy storage. Here, we propose a multilevel heterointerface engineering strategy that integrates boron nitride and barium niobate nanosheets through lattice interlocking. The large work\u2010function offset and bandgap contrast induce interfacial band bending and a built\u2010in electric field, forming a complementary trap\u2010barrier network that guides, blocks, and confines charge carriers. This design effectively suppresses charge injection and mobility, enhances interfacial polarization, and mitigates the propagation of breakdown pathways. Consequently, BNO@BN\/PEI composites achieve exceptional energy storage performance, delivering 9.02 J cm\n                    <jats:sup>\u22123<\/jats:sup>\n                    (\n                    <jats:italic>\u03b7<\/jats:italic>\n                    = 92%) at room temperature and sustaining 6.1 J cm\n                    <jats:sup>\u22123<\/jats:sup>\n                    (\n                    <jats:italic>\u03b7<\/jats:italic>\n                    \u2248 90%) at 150\u00b0C, while still preserving 4.6 J cm\n                    <jats:sup>\u22123<\/jats:sup>\n                    at 200\u00b0C. First\u2010principles calculations and finite element simulations further validate the structural and functional superiority of the multilevel heterointerface. This work establishes multilevel heterointerface engineering as a generalizable paradigm for breaking the trap\u2010barrier trade\u2010off in conventional dielectric design and paves the way for next\u2010generation high\u2010energy\u2010density and thermally robust polymer capacitors.\n                  <\/jats:p>","DOI":"10.1002\/adma.202517624","type":"journal-article","created":{"date-parts":[[2026,2,11]],"date-time":"2026-02-11T15:35:13Z","timestamp":1770824113000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Multilevel Heterointerface Engineering Breaks the Trap\u2010Barrier Trade\u2010Off in High\u2010Energy\u2010Density Polymer Dielectrics"],"prefix":"10.1002","volume":"38","author":[{"given":"Yang","family":"Liu","sequence":"first","affiliation":[{"name":"Electronic Materials Research Laboratory &amp; Multifunctional Materials and Structures Key Laboratory of the Ministry of Education &amp; International Center for Dielectric Research School of Electronic Science and Engineering Xi'an Jiaotong University  Xi'an Shaanxi China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhenjun","family":"Shao","sequence":"additional","affiliation":[{"name":"Electronic Materials Research Laboratory &amp; 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