This study investigated the effect of catalyst amount on chemical vapour deposition (CVD) growth of multi-walled carbon nanotubes (MWCNTs) with and without hydrogen feed. The ferrocene weight was varied from 100 mg to 200 mg for CNTs growth over Si/SiO2/Al2O3 substrate. Very few CNTs were seen in micrographs of the samples produced in the absence of the hydrogen feed. Most of the carbon atoms precipitated into amorphous carbon due to existence of inactive catalyst particles. However, CNT structures grown with hydrogen feed were more distinct; the nanotubes were thinner, straight and highly crystalline. MWCNTs arrays/forest length was also increased from 120 μm to 850 μm with hydrogen feed. An increase in catalyst weight significantly affected the diameter, crystallinity, alignment and growth of nanotubes. The lowest inner-shell spacing of 0.348 nm was obtained with 150 mg of ferrocene, which is an indication of growth of relatively pure CNTs. Under the optimum conditions, the areal density of the ferrocene particles was sufficiently increased to get required alignment and crystallinity of MWCNTs. © 2016 Trans Tech Publications, Switzerland.