Multiwalled carbon nanotubes (MWCNTs) have been grown on various substrates by thermal chemical vapordeposition using multilayered metal catalysts. Ion beam sputtering is used to deposit various metal layerssequentially. Underlayers of Al (2−20 nm) are shown to influence the growth characteristics with Fe or Niused as active catalysts. The as-sputtered catalyst surface, characterized using atomic force and scanningtunneling microscopies, consists of nanometer scale (<10 nm) catalyst particles. High-resolution transmissionelectron microscopy and Raman analysis are used to characterize the MWCNTs. Optimization of the twolayers allows growth of MWCNT towers on patterned and unpatterned substrates.