SrAl2O4: Eu2+ and Dy3+ phosphorescent phosphors were synthesized using the polymerized complex method. Generally, phosphorescent phosphors synthesized by conventional solid state reaction show a micro-sized particle diameter; thus, this process is restricted to applications such as phosphorescent ink and paint. However, it is possible to synthesize homogeneous multi-component powders with fine particle diameter by wet process such as the polymerized complex method. The characteristics of SrAl2O4: Eu2+ and Dy3+ powders prepared by polymerized complex method with one and two step calcination processes were comparatively analyzed. Temperatures of organic material removal and crystallization were observed through TG-DTA analysis. The crystalline phase and crystallite size of the SrAl2O4: Eu2+ and Dy3+ phosphorescent phosphors were analyzed by XRD. Microstructures and afterglow characteristics of the SrAl2O4: Eu2+ and Dy3+ phosphors were measured by SEM and spectrofluorometry, respectively.