A simple method is developed for the synthesis of carbon nanotubes (CNTs) using Mo-Co/MgO catalyst by a thermal chemical vapor deposition (CVD) technique. Acetylene was used as the source of carbon and nitrogen as carrier gas. A series of MgO supported Mo-Co catalysts were prepared by the combustion route using urea as the fuel at different stoichiometric ratios. It was found that a higher yield of carbon nanotubes was obtained by the developed catalysts. Also, the addition of molybdenum to Co/MgO catalysts could remarkably increase the yield and also improve the quality of CNTs from thermal CVD with acetylene as precursor gas. The morphology of the catalysts and CNTs obtained was studied by field emission scanning electron microscope (FE-SEM). Other techniques like Raman spectroscopy and XRD were also employed to know the physico-chemical properties of the samples.