The synthesis of bulk amounts of high quality single-walled carbon nanotubes (SWNTs) is accomplished by optimizing the chemical compositions and textural properties of the catalyst material used in the chemical vapor deposition (CVD) of methane. A series of catalysts are derived by systematically varying the catalytic metal compounds and support materials. The optimized catalysts consist of Fe/Mo bimetallic species supported on a novel silica-alumina multicomponent material. The high SWNT yielding catalyst exhibits high surface-area and large mesopore volume at elevated temperatures. Gram quantities of SWNT materials have been synthesized in similar to 0.5 h using the optimized catalyst material. The nanotube material consists of individual and bundled SWNTs that are free of defects and amorphous carbon coating. This work represents a step forward toward obtaining kilogram scale perfect SWNT materials via simple CVD routes.