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Abstract Vertically aligned carbon nanotube arrays (VACNTs) show a great potential for various applications, such as thermal interface materials (TIMs). Besides the thermally oxidized SiO2, atomic layer deposition (ALD) was also used to synthesize oxide buffer layers before the deposition of the catalyst, such as Al2O3, TiO2, and ZnO. The growth of VACNTs was found to be largely dependent on different oxide buffer layers, which generally prevented the diffusion of the catalyst into the substrate. Among them, the thickest and densest VACNTs could be achieved on Al2O3, and carbon nanotubes were mostly triple-walled. Besides, the deposition temperature was critical to the growth of VACNTs on Al2O3, and their growth rate obviously reduced above 650 °C, which might be related to the Ostwald ripening of the catalyst nanoparticles or subsurface diffusion of the catalyst. Furthermore, the VACNTs/graphene composite film was prepared as the thermal interface material. The VACNTs and graphene were proved to be the effective vertical and transverse heat transfer pathways in it, respectively.