Radiation possesses inherent physical characteristics, such as penetrability and radionuclide energy, which enable its widespread applicability in fields such as medicine, industry, environment, security, and research. Advancements in scintillator-based radiation detection technology have led to revolutionary changes by ensuring the safe use and precise measurement of radiation. Nevertheless, certain fields require higher scintillation yields to obtain more refined and detailed results. Therefore, in this study, we explored inorganic scintillators coated with perovskite nanomaterials to detect gamma rays with high light yields. By mixing perovskite with a polymer, we improved the intrinsic characteristics of quantum dots, which otherwise failed to maintain their performance over time. On this basis, we investigated the interactions among inorganic scintillators and a mixed material (CsPbBr3 + PMMA) and confirmed an increase in the scintillation yield and measurement trends. Furthermore, optimized scintillation yield measurement experiments facilitated gamma spectroscopy, demonstrating the validity of our approach through the analysis of the peak channel increases in the energy spectra of various gamma sources in relation to the increased scintillation yield.