As a leader of long persistent luminescence (LPL) materials, the optical properties of aluminate phosphor have remained unsurpassed for many years. As a powder material, its practical application will always be limited to the field of security signs. In this paper, the SrAl2O4:Eu2+, Dy3+ inorganic solid material with comparable LPL properties to powder materials was obtained. The crystallization mechanism and crystallite micro-morphology of inorganic glass materials have been studied, and a new opinion is put forward that the large-size SrAl2O4 crystallites in the glass matrix are stacked by rod-shaped crystals arranged in a regular direction. In addition, the SrAl2O4:Eu2+, Dy3+ glass obtained cannot only collect high-energy photons but also is sensitive to low-energy sunlight. The results show that the material exhibits superior performance in LPL, thermoluminescence, and photostimulable luminescence. Based on this property, a new application of this material in the field of information storage was explored. This paper has a certain reference value for the development and application of aluminate LPL materials in the field of smart optical information storage.