Discrete catalytic nanoparticles with diameters in the range of 1−2 nm and 3−5 nm respectively are obtained by placing controllable numbers of metal atoms into the cores of apoferritin, and used for growth of single-walled carbon nanotube (SWNTs) on substrates by chemical vapor deposition (CVD). Atomic force microscopy (AFM), transmission electron microscopy (TEM), and micro-Raman spectroscopy are used to characterize isolated nanotubes grown from the discrete nanoparticles. The characterizations, carried out at single-tube and single-particle level, obtain clear evidence that the diameters of nanotubes are determined by the diameters of catalytic nanoparticles. With nanoparticles placed on ultrathin alumina membranes, isolated SWNTs are grown and directly examined by transmission electron microscopy. For the first time, both ends of an as-grown single-walled nanotube are imaged by TEM, leading to a microscopic picture of nanotube growth mechanism. It is shown that controlling the structures of catalytic nanoparticles allows the control of nanotube diameter, and could also enable the control of SWNT length and eventually chirality.