The application of high throughput methodology in the discovery of catalyst formulations and novel nanomaterials is expected to impact a wide range of applications. Carbon nanomaterials such as nanotubes, nanofibers, and diamond-like carbon are promising candidate materials for use in a wide variety of electrical, optical and mechanical applications. Therefore, the application of combinatorial methodologies to the discovery and optimization of carbon nanomaterials and catalyst formulations to produce them will accelerate the advancement of nanoscale science and technology. Here, we present an overview of the various combinatorial methodologies employed in the search for carbon nanotubes and related structures. It is hoped that continued innovations in high throughput methodology, especially for nanomaterials development, would be adapted to the many challenges facing nanotechnology. (C) 2003 Elsevier Science B.V. All rights reserved.