Abstract: Carbon nanotubes were synthesized in a methane plasma by using Fe2O3/Ni as catalysis. Methane is pyrolyzed efficiently into nano-carbon and H2 by the plasma jet under atmospheric pressure, during which Fe2O3 is reduced by H2 to form nanometer sized metallic particles, which together with Ni are used as bimetallic catalysts for the preparation of nanotubes. The carbon nanotubes were examined using TEM and chemical element analysis, etc. Results show that the carbon nantotubes present an appearance of entangled morphologies with outer diameters of 10-30nm, length of several hundred nanometers, and the yield is about 75%. Compared with the single catalyst, the bimetallic catalyst is advantageous for the mass production of carbon nanotubes.