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Vertically aligned carbon nanotubes were synthesized on Ni-deposited Si substrates using microwave plasma-enhanced chemical vapor deposition. The grain size of Ni thin films varied with the rf power density during the rf magnetron sputtering process. We found that the diameter, growth rate, and density of carbon nanotubes could be controlled systematically by the grain size of Ni thin films. With decreasing the grain size of Ni thin films, the diameter of the nanotubes decreased, whereas the growth rate and density increased. High-resolution transmission electron microscope images clearly demonstrated synthesized nanotubes to be multiwalled. © 2000 American Institute of Physics.