CuInSe2 thin films were successfully prepared by selenization of precursor films coated on the Mo foils. The precursor films were compacted to improve surface morphology and density of CuInSe2 thin films. The films were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), and energy dispersive spectroscopy (EDS). The results indicate that the single-phase CuInSe2 is formed at 210 °C in selenization process and it exhibits preferred orientation along the (112) plane. The selenization temperature is above 210 °C, the selenization temperature rises to promote the crystallinity of selenized films, not to induce the occurrence of a new phase. The compact CuInSe2 film with smooth surface can be obtained by selenization of precursor films pressed with the pressure of 300 MPa.