The effects of Al3+ and crystallization heat treatment on the luminescence and radioluminescence properties of CsPbBr3 perovskite quantum dot borophosphate glass-ceramics were investigated using X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and Raman spectroscopy. Al3+ can suppress the free migration of ions in glass and control the formation of Pb–Br by improving the stability of the glass. Spectral analysis results revealed that small quantum dots are beneficial for achieving high-efficiency photoluminescence, whereas large microcrystals are beneficial for achieving high-efficiency radioluminescence. The experiment also proved that excessive Br− is not conducive to the precipitation of CsPbBr3 perovskite in glass and thus deteriorates the photoluminescence and radioluminescence properties of the glass.