The films of nanoscale-carbonare is formed through laser exfoliation of graphite on the substrate silicon (Si) without a catalytic layer and the chamber is vacuumed to 1.33×10-4 Pa in the growth process. The femtosecond (fs) laser exfoliation process is investigated at different laser fluences and deposition time. The composition of the carbon films deposited at different pulse energies and irradiation time are detected by the visible Raman spectroscopy. Scanning electron microscope (SEM) and atomic force microscope are used to display the surface of the thin films. The results show that the deposition time influences ratio of ID/IG, microstructure, the grain size of the carbon. High-intensity femtosecond laser pulse energy can promote the crystallization of carbon particles. Some special particles (pattern-snowflake-like，cube and quadrangle), which are formed by femtosecond laser pulse ablates a graphite at a high laser fluence, particles are found on the sample surface.