The effects of H-2 plasma pretreatment on the growth of vertically aligned carbon nanotubes (CNTs) by varying the flow rate of the precursor gas mixture during microwave plasma chemical vapor deposition (MPCVD) have been investigated in this study. Gas mixture of H-2 and CH4 with a ratio of 9:1 was used as the precursor for synthesizing CNTs on Ni-coated TiN/Si(1 0 0) substrates. The structure and composition of Ni catalyst nanoparticles were investigated by using scanning electron microscopy (SEM) and cross-sectional transmission electron microscopy (XTEM). Results indicated that, by manipulating the morphology and density of the Ni catalyst nanoparticles via changing the flow rate of the precursor gas mixture, the vertically aligned CNTs could be effectively controlled. The Raman results also indicated that the intensity ratio of the G and D bands (I-D/I-G) is decreased with increasing gas flow rate. TEM results suggest H-2 plasma pretreatment can effectively reduce the amorphous carbon and carbonaceous particles and. thus. is playing a crucial role in modifying the obtained CNTs structures. (c) 2007 Elsevier B.V. All rights reserved.