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Owing to the development of electronic devices moving toward high power density, miniaturization, and multifunction, research on thermal interface materials (TIMs) is become increasingly significant. Graphene is regarded as the most promising thermal management material owing to its ultrahigh in‐plane thermal conductivity. However, the fabrication of high‐quality vertical graphene (VG) arrays and their utilization in TIMs still remains a big challenge. In this study, a rational approach is developed for growing VG arrays using an alcohol‐based electric‐field‐assisted plasma enhanced chemical vapor deposition. Alcohol‐based carbon sources are used to produce hydroxyl radicals to increase the growth rate and reduce the formation of defects. A vertical electric field is used to align the graphene sheets. Using this method, high‐quality and vertically aligned graphene with a height of 18.7 µm is obtained under an electric field of 30 V cm−1. TIMs constructed with the VG arrays exhibit a high vertical thermal conductivity of 53.5 W m−1 K−1 and a low contact thermal resistance of 11.8 K mm2 W−1, indicating their significant potential for applications in heat dissipation technologies.
An alcohol‐based electric‐field‐assisted plasma enhanced chemical vapor deposition method is developed to grow vertical graphene (VG) arrays with high thermal conductivity. Using this method, high‐quality and vertically aligned graphene sheets at a height of 18.7 µm are obtained. Thermal interface materials constructed with these VG arrays exhibit excellent thermal properties for the heat dissipation of electrical devices.