This review article highlights the exploration of inorganic nanoscintillators for various scientific and technological applications in the fields of radiation detection, bioimaging, and medical theranostics. Various aspects of nanoscintillators pertaining to their fundamental principles, mechanism, structure, applications are briefly discussed. The mechanisms of inorganic nanoscintillators are explained based on the fundamental principles, instrumentation involved, and associated physical and chemical phenomena, etc. Subsequently, the promise of nanoscintillators over the existing single-crystal scintillators and other types of scintillators is presented, enabling their development for multifunctional applications. The processes governing the scintillation mechanisms in nanodomains, such as surface, structure, quantum, and dielectric confinement, are explained to reveal the underlying nanoscale scintillation phenomena. Additionally, suitable examples are provided to explain these processes based on the published data. Furthermore, we attempt to explain the different types of inorganic nanoscintillators in terms of the powder nanoparticles, thin films, nanoceramics, and glasses to ensure that the effect of nanoscience in different nanoscintillator domains can be appreciated. The limitations of nanoscintillators are also highlighted in this review article. The advantages of nanostructured scintillators, including their property-driven applications, are also explained. This review article presents the considerable application potential of nanostructured scintillators with respect to important aspects as well as their physical and application significance in a concise manner.