The structure phase transformations of graphite and carbon black induced by pulsed laser were studied in this paper. Under irradiation with laser beam of 1.06μm wavelength and power density of 106 W· cm- 2, both graphite structure and carbon black structure were changed obviously. The results of Raman analyses and Transmission Electron Microscopy (TEM) observations show that graphite transforms into nanodiamond about 5 nm and carbon black is graphitized. It is demonstrated that graphite is the intermediate phase in the transformation from carbon black to diamond, and graphite is easier to transform into diamond by laser irradiation than carbon black.