The synthesis of Ni-catalyzed multi-walled carbon nanotubes and nanofibers on a catalytic metal substrate, using an ethylene fueled inverse diffusion flame as a heat source, was investigated. When the gas temperature was varied from 1,400K to 900K, approximately, carbon nanotubes with diameters of 20∼60nm were formed on the substrate. In the regions where the gas temperature was higher than 1,400K or lower than 900K, iron nanorods or carbon nanofibers were synthesized, respectively. Based on the quantitative analyses of large amount of SEM and TEM images, the nanotubes formed closer to the flame had a tendency of having larger diameters. HR-TEM images and Raman spectra revealed that carbon nanotubes synthesized had multi-walled structures with some defective graphite layers at the wall. Based on the graphite mode of the Raman spectra, it was believed that the optimal synthesis could be obtained as the substrate was positioned at between 5.5mm and 5.0mm, from the flame axis.