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Vertically aligned carbon nanotube (VACNT) arrays are considered a promising candidate for a thermal interface material (TIM) due to their good stability, high thermal conductivity, and desirable mechanical properties. In the last few decades, extensive studies have been performed on the preparation and properties of VACNT arrays for TIM applications. In this perspective, we introduce recent progress on improving the intrinsic thermal conductivity, decreasing the thermal contact resistance, and the efficient transfer of VACNT arrays, then discuss challenges that need to be overcome, and predict the future of VACNT-based TIMs.