A series of phosphor layers (ZnS:Cu‐Large, ZnS:Cu‐Small, and Y2O2S:Eu) precipitated with varying mass thicknesses were prepared using a homogeneous precipitation method. Radioluminescence (RL), the light emitted from phosphor materials immediately upon beta particle radiation, was measured at room temperature using RL spectra under 4.89 mCi cm−2 63 Ni and 2.23 mCi cm−2 147 Pm beta particle sources, respectively. The RL properties, such as emission intensity, are affected by the mass thickness of the phosphor layers. In this work, the performance of beta‐radioluminescent nuclear batteries with the aforementioned phosphor layers as intermediate absorbers was analyzed and discussed. The current–voltage characteristics of the nuclear batteries revealed the effect of the physical parameters of the phosphor layers. The maximum output power of the batteries increased approximately linearly with increasing RL intensity for the three types of phosphors under excitation by different beta sources.