A catalyst material for carbon nanotube synthesis includes a uniform dispersion of host particles on a substrate. The host particles themselves include catalyst nanoparticles that are effective to catalyze nanotube syntheses reactions and provide nucleation sites. Methods for preparing catalyst materials include co-sputtering a catalytic species and a host species to form a precursor thin film on a substrate, followed by an oxidation reaction of the precursor thin film in air. The precursor thin film can be patterned on the substrate to limit the locations of the catalyst material to well-defined areas. Methods for nanotube synthesis employ CVD in conjunction with the catalyst materials of the invention. During the synthesis, the catalyst nanoparticles catalyze carbon nanotubes to grown from a carbon-containing gas.