At present, extensive studies on the synthesis of aligned carbon nanotubes (CNTs) are being carried out in order to determine the optimum characteristics required for applications in nanodevices. Past researches have shown that the growth of the CNTs is highly dependant on the catalyst used. The more common types of catalyst used are Ni, Fe, Co and metal alloys of these elements. Usually, the precursor of the catalysts used is either metal salts (together with support and calcined to form crystalline structure) or in solid form (using physical deposition method). The first method usually results in bulk CNTs while the later will produce vertically aligned CNTs film. However, not much work has been reported on the use of metal powder as the catalytic source. The objective of this work is to study and compare the crystallinity and morphology of the CNTs obtained via thermal CVD growth method, using Fe powder and pellet. Analyses performed include Raman spectroscopy and scanning electron microscopy (SEM). Although SEM images seem to indicate that the film thickness and overall morphology of the CNTs obtained in both setup are similar, the crystallinity of CNTs obtained with Fe pellets are better compared to those achieved using Fe powder. © 2009 American Institute of Physics.