The Fe(CO) 5 catalyzed pyrolysis of pentane was investigated. The study, performed in a quartz tube, revealed that a range of carbonaceous materials could be formed with products determined by the temperature profile in the tube, the Fe(CO) 5 content in pentane, the carrier gas flow rate, the pyrolysis temperature and the pyrolysis time. The distribution of carbonaceous products also depends on the competition of the pyrolysis of Fe(CO) 5 and pentane in the different regions of the reactor. Carbonaceous materials produced included graphite film, carbon nanotubes and carbon nanoballs. The formation of carbon nanotubes takes place in a region in the quartz tube where both the pyrolysis of both Fe(CO) 5 and pentane occur, with carbon nanotubes formed by the pyrolysis of pentane. Alignment of carbon nanotubes was found when a high Fe(CO) 5 concentration was used.