A film formation is performed using a target in which a material which is volatilized more easily than gallium when heated at 400° C. to 700° C., such as zinc, is added to gallium oxide by a sputtering method with high mass-productivity which can be applied to a large-area substrate, such as a DC sputtering method or a pulsed DC sputtering method. This film is heated at 400° C. to 700° C., whereby the added material is segregated in the vicinity of a surface of the film. Another portion of the film has a decreased concentration of the added material and a sufficiently high insulating property; therefore, it can be used for a gate insulator of a semiconductor device, or the like.