In the current work, we show that it is possible to favor the selective growth of single-walled carbon nanotubes (SWCNTs) with a narrow diameter distribution on supported catalyst particles with a broad size distribution. Carbon nanotubes were grown at 600 °C on silicon substrates. The structure of carbon deposits was controlled by managing the carbon feedstock for adjusting the rate of carbon nanostructures formation on the surface of catalyst particles. Either carbon nanofibers (CNFs) carpets or isolated SWCNTs were obtained. With the fine tune of carbon feedstock, small isolated SWCNTs with a narrow diameter distribution were obtained by limiting the catalytic activity of the largest catalyst particles. HRTEM observations of nanotube embryos have suggested a possible mechanism of multi-walled carbon nanotubes (MWCNTs) formation that can explain why the growth of MWCNTs with parallel walls seems to be more difficult than SWCNTs or CNFs at low temperature.