In this study, Fe/MgO catalysts with three different iron contents (5, 10, and 15 wt.%) were prepared by three catalyst preparation methods: impregnation, solution combustion synthesis, and co-calcination of metal nitrates. The resulting catalysts were subjected to methane at 900°C in order to grow carbon nanotubes (CNTs). The powders and products were then studied by X-ray diffraction (XRD), differential thermal analysis (DTA), scanning and transmission electron microscopy (SEM and TEM), and Raman spectroscopy. Formation of MgFe 2 O 4 upon heating the catalysts to 900°C was confirmed by XRD. After the growth step, corresponding peaks of MgFe 2 O 4 disappeared and metallic iron peaks appeared, indicating that MgFe 2 O 4 is the responsible phase for production of iron nanoparticles. HRTEM images showed that the product on the 5 wt.% catalysts was mostly SWNTs and DWNTs with no evidence of carbon nanofibres or multi-walled carbon nanotubes on the co-calcination catalyst. Furthermore, I D /I G ratios obtained from Raman spectra were all below 0.1, except for one sample, showing the good quality of the products.