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The isoelectronic diamond and boron nitride (BN) can present both cubic and wurtzite polymorphs and hence prospectively form diverse heterostructures. However, synthesizing the metastable hexagonal diamond\/wurtzite BN (HD\/wBN) covalent heterostructures and clarifying the interfacial chemical bonds remain great challenges, despite considerable effort. In this study, we have demonstrated the direct synthesis of high\u2010quality HD\/wBN covalent heterostructures via structural transformation of graphite\/hBN vdW heterostructures under high pressure and high temperature. Raman and structural characterizations evidently confirmed the sharp HD\/wBN heterointerface with both C\u2500B and C\u2500N bonds, attributed to inversion domain boundaries within the wBN phase. The mapped pressure\u2010temperature diagram exhibited the confined window required for HD\/wBN heterostructures. Our work provides a viable pathway to prepare various covalent heterostructures through synergistic phase transitions and opens new opportunities for exploring their pronounced properties.<\/jats:p>","DOI":"10.1002\/adma.74216","type":"journal-article","created":{"date-parts":[[2026,7,22]],"date-time":"2026-07-22T14:05:09Z","timestamp":1784729109000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Controlled Synthesis and Interfacial Bonding of Hexagonal Diamond\/Wurtzite Boron Nitride Covalent Heterostructures"],"prefix":"10.1002","volume":"38","author":[{"ORCID":"https:\/\/orcid.org\/0009-0005-6193-7205","authenticated-orcid":false,"given":"Lu","family":"Bai","sequence":"first","affiliation":[{"name":"School of Interdisciplinary Science Beijing Institute of Technology  Beijing China"},{"name":"School of Chemistry and Chemical Engineering Beijing Institute of Technology  Beijing 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