The dehydrogenation thermodynamics and kinetics of hydrogen-storage materials are critical for their applications in solid propellants. In this paper, the effects of nanosizing on dehydrogenation thermodynamics and kinetics of various categories of hydrogen-storage materials were systematically reviewed. It is revealed that the nanoscale chemical hydrogen-storage materials possess lower dehydrogenation temperatures and better dehydrogenation kinetics in comparison with their bulk counterparts, which is favorable for the full utilization of their hydrogen during the combustion of solid propellants. On the other hand, the nanoscale chemical-physical hydrogen-storage materials can be adopted as both hydrogen sources and combustion catalysts for propellants. In addition, it is believed that modifications in structural characteristics of nanoscale physical hydrogen-storage materials can enable them to dehydrogenate/hydrogenate fast at room temperature, illustrating their great potential as hydrogen sources for solid propellants. The key point for development of practical nanoscale hydrogen-storage materials as hydrogen sources for propellants is to determine the optimal thermodynamics and kinetics parameters for the applications, which are crucial for the design and preparation of nanoscale hydrogen-storage materials for propellants.