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Here, we transcend conventional surface modification by introducing a phase\u2010engineering strategy to fundamentally reconfigure the AlN surface. Through fluidized bed\u2010chemical vapor deposition, we precisely construct conformal, high\u2010crystalline and low\u2010defective graphene \u201cskin\u201d on AlN powders (the intensity ratio of D\u2010peak to G\u2010peak \u223c0.088), where the unique growth kinetics and interfacial phase are dictated by the AlN substrate, thus differ from the conventional non\u2010metallic substrates. As revealed by density functional theory calculations, this process yields a covalently\u2010bonded heterointerface characterized by distinct C\u2013Al\u2013N configurations, thereby moving beyond weak van der Waals interactions. The phase\u2010engineered graphene skin delivers dual, synergistic functions, enhancing the thermal conductivity of AlN by 38.7% via optimized thermal transport pathways, while simultaneously acting as an ultrastable barrier, granting exceptional resistance to prolonged hygrothermal aging with the thermal conductivity variation of thermal interface material less than 1% in 30 days. This work resolves the long\u2010standing trade\u2010off between environmental stability and thermal performance in AlN, establishing a paradigm of phase\u2010engineered graphene encapsulation for ceramic fillers, thereby enabling the scalable fabrication of robust, hydrolysis\u2010resistant and high thermal conductivity composites.<\/jats:p>","DOI":"10.1002\/adma.202523695","type":"journal-article","created":{"date-parts":[[2026,3,11]],"date-time":"2026-03-11T14:35:50Z","timestamp":1773239750000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Concurrent Hydrolysis Resistance and High Thermal Conductivity in Aluminum Nitride Enabled by Phase\u2010Engineered Graphene Encapsulation"],"prefix":"10.1002","author":[{"given":"Yuzhu","family":"Wu","sequence":"first","affiliation":[{"name":"Center for Nanochemistry Beijing Science and Engineering Center for Nanocarbons Beijing National Laboratory for Molecular Science College of Chemistry and Molecular Engineering Peking University  Beijing P. R. China"},{"name":"Beijing Graphene Institute (BGI)  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yueming","family":"Hu","sequence":"additional","affiliation":[{"name":"Beijing Graphene Institute (BGI)  Beijing P. R. China"},{"name":"Academy for Advanced Interdisciplinary Studies Peking University  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qiuyue","family":"Zhang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Precision and Intelligent Chemistry University of Science and Technology of China  Hefei P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ziyue","family":"Xu","sequence":"additional","affiliation":[{"name":"Academy for Advanced Interdisciplinary Studies Peking University  Beijing P. R. China"},{"name":"Electron Microscopy Laboratory School of Physics Peking University  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaopan","family":"Qiu","sequence":"additional","affiliation":[{"name":"Beijing Graphene Institute (BGI)  Beijing P. R. China"},{"name":"Zhongyuan Graphene Laboratory  Zhengzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Haonan","family":"Zhai","sequence":"additional","affiliation":[{"name":"Beijing Graphene Institute (BGI)  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhifeng","family":"Sun","sequence":"additional","affiliation":[{"name":"Beijing Graphene Institute (BGI)  Beijing P. R. China"},{"name":"State Key Laboratory of Organic\u2010Inorganic Composites College of Materials Science and Engineering Beijing University of Chemical Technology  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jingyang","family":"Chen","sequence":"additional","affiliation":[{"name":"Beijing Graphene Institute (BGI)  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dan","family":"Li","sequence":"additional","affiliation":[{"name":"Beijing Graphene Institute (BGI)  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuqi","family":"Xia","sequence":"additional","affiliation":[{"name":"Beijing Graphene Institute (BGI)  Beijing P. R. China"},{"name":"State Key Laboratory of Chemical Resources Engineering Beijing Key Laboratory of Electrochemical Process and Technology for Materials Beijing University of Chemical Technology  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wenhu","family":"Wang","sequence":"additional","affiliation":[{"name":"Beijing Graphene Institute (BGI)  Beijing P. R. China"},{"name":"State Key Laboratory of Heavy Oil Processing College of Science China University of Petroleum  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ali","family":"Cai","sequence":"additional","affiliation":[{"name":"Beijing Graphene Institute (BGI)  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Peng","family":"Gao","sequence":"additional","affiliation":[{"name":"Academy for Advanced Interdisciplinary Studies Peking University  Beijing P. R. China"},{"name":"Electron Microscopy Laboratory School of Physics Peking University  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhenyu","family":"Li","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Precision and Intelligent Chemistry University of Science and Technology of China  Hefei P. R. 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