In this study, we investigate the effect of the diffusion barrier and substrate temperature on the length of carbon nanotubes. For synthesizing vertically aligned carbon nanotubes, thermal chemical vapor deposition is used and a substrate with a catalytic layer and a buffer layer is prepared using an e-beam evaporator. The length of the carbon nanotubes synthesized on the catalytic layer/diffusion barrier on the silicon substrate is longer than that without a diffusion barrier because the diffusion barrier prevents generation of silicon carbide from the diffusion of carbon atoms into the silicon substrate. The deposition temperature of the catalyst and alumina are varied from room temperature to 150°C, 200°C, and 250°C. On increasing the substrate temperature on depositing the buffer layer on the silicon substrate, shorter carbon nanotubes are obtained owing to the increased bonding force between the buffer layer and silicon substrate. The reason why different lengths of carbon nanotubes are obtained is that the higher bonding force between the buffer layer and the substrate layer prevents uniformity of catalytic islands for synthesizing carbon nanotubes.