The temperature and time dependences of carbon nanotube (CNT) growth by chemical vapor deposition are studied using a multilayered Al/Fe/Mo catalyst on silicon substrates. Within the 600–1100 °C temperature range of these studies, narrower temperature ranges were determined for the growth of distinct types of aligned multi-walled CNTs and single-walled CNTs by using high-resolution transmission electron microscopy and Raman spectroscopy. At 900 °C, in contrast to earlier work, double-walled CNTs are found more abundant than single-walled CNTs. Defects also are found to accumulate faster than the ordered graphitic structure if the growth of CNTs is extended to long durations.