Photoluminescent SrAl2O4:Eu,Dy thin films were successfully prepared by a pulsed ion-beam evaporation method without substrate heating or sample annealing. The crystallinity of the films was observed by X-ray diffraction and large-area high-resolution electron microscopy. From the above results and photoluminescence spectra (PL), it was concluded that the intensity at the peak in PL spectra is related to the volume fraction of a crystallized SrAl2O4,:Eu,Dy phase in the thin films.