The rapid development of radioluminescent nanomaterials has left uncertainties in how their properties compare to bulk materials or other luminescent nanoparticles. The effects of material density and effective atomic number, activator concentration, co-doped sensitization, and core/ shell architectures were examined, with a focus on LiLuF 4 nanoparticles doped with Eu 3+ . Varying material density and effective atomic number were found to affect the exciton recombination efficiency and subsequent excitation of activator ions. Given the indirect excitation processes in radioluminescence, we observed that the dependence on dopant concentration is highly specific to the choice of the activator ion and host composition. Strategies to enhance the radioluminescence efficiency were explored through co-doping with a sensitizer ion or core/shell architectures. Demonstrated herein, co-doping is a viable strategy to improve radioluminescence; however, the effect is highly dependent on the sensitizer−activator ion combination, as well as the population efficiency of the sensitizer. Core/shell structures were effective in improving the efficiency of individual activator ions in the lattice; however, the enhancement may not compensate for the addition of nonluminescent shell material. The results provide insight on the development of radioluminescent nanoparticles and their relationship to the properties that govern other luminescence processes.