ZrCo alloy has been initially applied in nuclear fusion experimental reactor due to its high hydrogen isotope storage capacity, low equilibrium pressure at room temperature and no radioactivity. However, ZrCo alloy has some issues, such as long activation time, poor kinetic properties and easy disproportionation, which restrict its engineering process. Therefore, it is of great significance to improve the hydrogen storage performance of ZrCo alloy and realize the synchronous improvement of dynamic characteristics, cycle stability and anti-disproportionation performance, which is crucial for revealing hydrogen storage mechanism of ZrCo alloy and promoting its engineering application. This review summarizes recent progress on nanostructural ZrCo alloys, especially the fact that nanostructural ZrCo alloy particles can shorten the activation time to less than 10 s, effectively improve the hydrogen absorption kinetics, and enhance the anti-disproportionation ability by more than 50% at 500 ℃, significantly improving the comprehensive hydrogen storage performance of ZrCo alloys. In this paper, the latest research trends of nanostructural ZrCo alloys are systematically summarized, and the mechanism of nanostructure on improving hydrogen storage performance is emphatically elaborated. The future research and application prospects of nanostructural ZrCo-based hydrogen storage isotope alloys are prospected.