Hydrogen storage is one of the most significant research areas for exploiting hydrogen energy economy. To store hydrogen with a high gravimetric/volumetric density, gaseous hydrogen storage systems require a very high-pressure compressed gas cylinder which is quite unsafe and the storage in the liquid form needs cryogenic containers to be maintained at roughly 20 K under ambient pressure because hydrogen has a very low critical temperature of 33 K. However, hydrogen can be stored in solid materials with higher concentration of hydrogen compared to the gaseous and liquid hydrogen storage systems. It is therefore, worthwhile to look into the experimental and theoretical research on prospective hydrogen storage materials. The hydride-forming alloys and intermetallic compounds are found to be the most important families of hydrogen storage materials. Multicomponent alloys consisting of five or more principal elements, also known as high-entropy alloys appear to have potential for the development as hydrogen storage materials. Hydride-forming elements like Ti, Zr, V, Nb, Hf, Ta, La, Ce, Ni, and others have been shown to have hydrogen storage properties and the ability to produce single-phase high-entropy intermetallics. Here, attempts will be made to present a short review on utilization of multicomponent high-entropy alloys as solid hydrogen storage materials. Furthermore, we will also present some of our work on the synthesis, structural–microstructural characterization and hydrogen storage properties of Ti–Zr–V–Cr–Ni equi-atomic hydride-forming high-entropy alloys. From the preliminary investigation, the maximum storage capacity in this system was observed to be 1.78 wt%, which is comparable to other hydrogen storage materials. The prospects of high-entropy-based alloys for hydrogen storage will be discussed.