Carbon nanotubes (CNTs) have been synthesized through chemical vapor deposition in argon gas atmosphere using Fe-2.5%Mo alloyed nanoparticles as a catalyst and H2/CH4 gas mixture as a reaction gas. Fe-2.5 wt.%Mo alloyed nanoparticles with average diameter of 7, 20, 45 and 85 nm are prepared by the chemical vapor condensation process using the pyrolysis of iron pentacarbonyl (Fe(CO)5) and molybdenum hexacarbonyl (Mo(CO)6). The morphologies of the CNTs are controlled by adjusting the nanoparticle size, reaction gas ratio and reaction temperature. With decreasing nanoparticle size under the same experimental conditions, the degree of crystalline perfection increases gradually and the morphologies of the carbon nanotubes vary from multi wall carbon nanotubes to single wall carbon nanotubes. Also, the ratio of reaction gas has an effect on the morphology and the degree of crystallinity of CNTs. In this work, it is suggested that morphology, diameter and degree of crystallinity of CNTs could be controlled by adjusting the reaction gas ratio, reaction temperature and catalyst size.