Alumina supported cobalt-ferrum catalysts were prepared using wet impregnation method by applying 3 different conditions, namely hotplate (A), sonication (B) and soaking (C). The alumina supported cobalt-ferrum catalysts were applied in the synthesis of multi-walled carbon nanotubes (MWNTs) using catalytic chemical vapour deposition (CCVD) technique. The morphology and particle size of the cobalt-ferrum catalysts and the MWNTs yield were examined by field emission-scanning electron microscopy (FE-SEM) while the surface elemental composition of the samples was obtained by energy dispersive X-ray analysis (EDX). The morphology of catalysts A, B and C were found to be different, the particle sizes were ranged from 20-40 nm. The diameters of the MWNTs yield from samples A, B and C were found to be related to the catalyst particle size, thus the smaller the catalyst particle, the thinner the MWNTs obtained. The MWNTs with smaller diameter were obtained with higher purity and quality becuase the nanotube surface are free from amorphous carbon. Therefore, different catalyst preparation methods resulted in different sizes of the catalyst particle in order to synthesize MWNTs with desired diameter.