Optically stimulated luminescence (OSL) materials, enabling energy storage by capturing of charge carriers and then the energy conversion to light via photostimulation, can find many advanced applications in various fields, spanning from radiation dosimetry, optical data storage and security, environmental monitoring, biomedicine, clinical diagnostic, to archaeology and geology. At present, there are some blocks, including the development of nanocrystallization approaches, the tailoring of optical transitions, the control of trap distribution, and the understanding of OSL mechanisms, on the road to the exploration of OSL materials. This review gives an overview of the design, preparation, characterization, optimization, application, mechanism, and prospect of OSL materials. A short introduction of the fundamental principle and history of OSL materials is presented, followed by a summary of preparation and design methods, and a survey of OSL materials reported to date. The trap engineering, mechanism, and study methodologies of OSL are summarized, after which the widespread applications of OSL materials, in traditional and newly emerging fields, are reviewed. Finally, the merits and drawbacks of the OSL materials according to the relevant reports currently available are examined. The challenges and outlooks are highlighted and discussed in terms of five important aspects that merit future research.