Electrodeposition is an excellent method for a site-selective and direct fabrication of catalyst nanoparticles for subsequent carbon nanotube (CNT) growth. Nickel nanoparticles with densities as high as 10(11) cm(-2) and diameters down to 15 +/- 4 nm are deposited on blanket and patterned TiN wafers. Ni nanoparticles are selectively placed at the bottom of submicrometer vias by through-mask electrodeposition. The spherical nanoparticles all produce aligned multiwalled CNTs. The CNT diameter is directly determined by the diameter of the as-deposited nanoparticles, which is tailored by the electrodeposition conditions. Such control of CNT size, density, and location represents an important step toward the implementation of CNTs in device fabrication.