We synthesized a 0.1% Li-doped ZnO translucent ceramic using spark plasma sintering (SPS) and annealed it at 700 or 800 °C in air. The photoluminescence (PL) and scintillation properties of all samples were evaluated. The PL quantum yield (QY) and scintillation light yield (LY) were improved by annealing owing to the reduction in the number of oxygen defects in comparison with the as-prepared sample. Among the translucent ceramic samples, the sample annealed at 700 °C showed the highest LY (5800 ph/5.5 MeV-α); the scintillation LY was lower in the sample annealed at 800 °C because of the increase in the number of trap sites.