Designing efficient electrocatalysts for efficient hydrogen evolution is extremely desired but challenging. Herein, we report a facile MOF-assisted strategy to synthesize the hierarchical hollow spherical NiRu-C nanohybrid with closely packed rod-like bulges on the surface. Benefited from the more exposed active sites of NiRu-C nanohybrid and the efficient electron/mass transport in its unique hierarchical hollow spherical nanostructure, the optimized nanohybrid showed excellent performance for alkaline hydrogen evolution with ultralow overpotentials, which are much superior to those of Pt/C and the overwhelming majority of reported electrocatalysts. The interpretation of the reaction mechanism was further discussed with DFT calculations. Our research may provide a guidance for the development of advanced electrocatalysts with controlled morphology and excellent performance for future energy applications.