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Herein, a soluble fluoroalkyl end\u2010capped polyimide (FPI) precursor is developed. The amphipathic structure of FPI acts as an intermolecular bridge, facilitating the homogeneous dispersion of hydrophobic hBN within aqueous PTFE emulsions. Upon thermal imidization, in situ microphase \u201crivet\u201d architectures evolve at the filler\u2010matrix boundaries, replacing fragile van der Waals contacts with robust, mechanically anchored transitional zones. The topological interlocking significantly restricts the long\u2010range segmental mobility of PTFE chains, yielding an exceptional thermal conductivity of 2.89\u00a0W\/m\u00b7K (a 7.5\u2010fold increase) alongside an ultralow copper\u2010matched coefficient of thermal expansion (12\u00a0ppm\/K). Remarkably, these breakthroughs are achieved while preserving superior dielectric properties (permittivity D\n                    <jats:sub>k<\/jats:sub>\n                    = 2.52, loss tangent D\n                    <jats:sub>f<\/jats:sub>\n                    = 0.00078 @ 10\u00a0GHz). This work establishes a universal and scalable blueprint for fabricating extreme\u2010performance PTFE substrates tailored for the stringent demands of next\u2010generation 5G\/6G telecommunications.\n                  <\/jats:p>","DOI":"10.1002\/adma.73747","type":"journal-article","created":{"date-parts":[[2026,6,19]],"date-time":"2026-06-19T09:00:54Z","timestamp":1781859654000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Microphase Rivet\u2010Reinforced Interfaces in PTFE Composites: Enabling High Thermal Conductivity and Dimensional Stability for High\u2010Frequency Substrates"],"prefix":"10.1002","volume":"38","author":[{"given":"Hanyu","family":"Guo","sequence":"first","affiliation":[{"name":"State Key Laboratory of Advanced Polymer Materials Polymer Research Institute of Sichuan University Sichuan Provincial Engineering Research Center of Plastic\/Rubber Complex Processing Technology  Chengdu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Renke","family":"Li","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Advanced Polymer Materials Polymer Research Institute of Sichuan University Sichuan Provincial Engineering Research Center of Plastic\/Rubber Complex Processing Technology  Chengdu China"},{"name":"Luzhou North Cellulose Co., Ltd.  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Luzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rong","family":"Chen","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Advanced Polymer Materials Polymer Research Institute of Sichuan University Sichuan Provincial Engineering Research Center of Plastic\/Rubber Complex Processing Technology  Chengdu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9972-0873","authenticated-orcid":false,"given":"Hong","family":"Wu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Advanced Polymer Materials Polymer Research Institute of Sichuan University Sichuan Provincial Engineering Research Center of Plastic\/Rubber Complex Processing Technology  Chengdu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shaoyun","family":"Guo","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Advanced Polymer Materials Polymer Research Institute of 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