The vanadium oxide thin films are prepared on zinc selenide by DC magnet sputtering method. The optical character changing of vanadium oxide thin films are tested by CO 2 laser, some phenomena is observed. The components are gotten by The X-ray photoelectron spectroscopy (XPS). By utilizing the Castep program package of the Material Studio simulation tool, based on local density function approximation and pseudo-potential method, optimization for the geometric structure of vanadium dioxides is accomplished with the BFGS calculate way. Using the super soft pseudo-potential of reciprocal space lattice, the optical characteristics of crystal are calculated within the 7 μm scope. Furthermore, some trends can be concluded from the extended estimation for the optical characteristics at 10.6 μm by formula.