Chemical vapor deposition (CVD) growth of carbon nanotubes directly on nickel substrates was carried out at different temperatures. Effects of temperature on the growth of carbon nanotubes were investigated and the nucleation and growth mechanism of carbon nanotubes at different temperature ranges were also discussed. Based on the growth mechanism of nanotubes, small amount of Fe nanoparticles were deposited on the nickel substrate to introduce more nucleation sites at elevated temperature, and the density of nanotubes on the surface of the substrate was greatly improved.