We have developed a novel method to grow carbon nanotubes in a periodic structure using a simple one-step self-assembly process. In this approach, monodispersed nanospheres are utilized to assemble smaller nanoparticle catalysts into an ordered periodic pattern. Using this process, we have grown carbon nanotube bundles into a honeycomb structure. The proposed method eliminates the need for lithography and material deposition, greatly reducing the fabrication complexity and cost.