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Graphene as a wonderful additive is often added into polymer to build composite TIMs. However, owing to the lack of a specific design of the graphene skeleton, thermal conductivity of graphene\u2010based composite TIMs is not significantly improved. Here a chloroform\u2010assisted method for rapid growth of vertical graphene (VG) arrays in electric field\u2010assisted plasma enhanced chemical vapor deposition (PECVD) system is reported. Under the optimum intensity and direction of electric field and by introducing the highly electronegative chlorine into the reactor, the record growth rate of 11.5\u00a0\u00b5m\u00a0h<jats:sup>\u22121<\/jats:sup> is achieved and VG with a height of 100\u00a0\u00b5m is successfully synthesized. The theoretical study for the first time reveals that the introduction of chlorine accelerates the decomposition of methanol and thus promotes the VG growth in PECVD. Finally, as an excellent filler framework in polymer matrix, VG arrays are used to construct a free\u2010standing composite TIM, which yields a high vertical thermal conductivity of 34.2\u00a0W\u00a0m<jats:sup>\u22121<\/jats:sup>\u00a0K<jats:sup>\u22121<\/jats:sup> at the graphene loading of 8.6\u00a0wt% and shows excellent cooling effect in interfacial thermal dissipation of light emitting diode.<\/jats:p>","DOI":"10.1002\/advs.202200737","type":"journal-article","created":{"date-parts":[[2022,3,24]],"date-time":"2022-03-24T20:10:51Z","timestamp":1648152651000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":48,"title":["Chloroform\u2010Assisted Rapid Growth of Vertical Graphene Array and Its Application in Thermal Interface Materials"],"prefix":"10.1002","volume":"9","author":[{"given":"Shichen","family":"Xu","sequence":"first","affiliation":[{"name":"Center for Nanochemistry Beijing Science and Engineering Center for Nanocarbons Beijing National Laboratory for Molecular Sciences College of Chemistry and Molecular Engineering Peking University  Beijing 100871 P. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Cheng\u2010Te","family":"Lin","sequence":"additional","affiliation":[{"name":"Key Laboratory of Marine Materials and Related Technologies Zhejiang Key Laboratory of Marine Materials and Protective Technologies Ningbo Institute of Materials Technology and Engineering (NIMTE) Chinese Academy of Sciences  Ningbo 315201 P. R. 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