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Vertically aligned carbon nanotubes (VACNTs) grown on bulk copper substrate are of great importance for real-life commercial applications of carbon nanotubes (CNTs) as thermal interface materials in microelectronic packaging. However, their reproducible syntheses have been a great challenge so far. In this study, by introducing a well-controlled conformal Al2O3 support layer on the bulk copper substrate by atomic layer deposition, we reproducibly synthesized VACNTs of good alignment and high quality on the copper substrate. The alignment and the quality were characterized by scanning electron microscope, transmission electron microscope, and Raman spectroscopy. The key roles of the conformal Al2O3 support layer by atomic layer deposition are discussed. This progress may provide a real-life VACNT application for thermal management.