Single-walled carbon nanotubes of uniform diameter were grown in cobalt-substituted MCM-41 molecular sieves templated with C12 and C16 alkyl chains to result in pore diameters of 2.6 and 3.3 nm, respectively. The narrow diameter distribution of the tubes grown was probed by Raman, UV-visible, and NIR spectroscopy, as well as by high-resolution transmission electron microscopy. Tube diameters have been observed to vary with the size of the Co clusters formed during carbon deposition, as measured by extended X-ray absorption fine structure (EXAFS). It is proposed that the diameter of the carbon nanotubes grown in MCM-41 catalysts is controlled by the size of the metallic clusters formed in the template. Because MCM-41 catalysts of different pore diameter form Co clusters of different sizes, this mechanism can be exploited to grow carbon nanotubes of uniform, preselected diameters.As widely reported, 1-5 carbon nanotubes exhibit technologically important electronic properties potentiating new device development. They can be found in both metallic and semiconducting structures. The structure of the single-walled nanotube (SWNT) is defined by how the graphitic sheet is aligned in the rolled up configuration. Metallic (m) nanotubes can carry extremely large current densities; 6 semiconducting (s) nanotubes can be electrically switched on and off as field-effect transistors (FETs) (e.g., ref 6). Most electronic applications of carbon nanotubes require aligned SWNTs that are reasonably homogeneous in diameter, length, and electronic properties. Odom et al. 7 used scanning tunneling microscopy (STM) to correlate atomic structure with electronic properties of SWNTs. They found that the electronic properties correlate both with the diameter and helicity (twist). This important work illustrates why control of SWNT diameter and structure is of crucial importance for the development of new electronic devices based on SWNTs.