Highly uniform vertical carbon nanotube arrays were prepared by a novel hybrid approach combining a plasma-enhanced chemical vapor deposition (PECVD) process with self-assembled block copolymer nanotemplate. Monodisperse catalyst nanoparticles were prepared on a substrate using self-assembled nanoporous block copolymer templates. The subsequent PECVD growth of vertical CNTs from the nanopatterned catalyst particles provided highly oriented vertical CNT arrays, which are potentially useful for device integration of CNTs.