Ruthenium (Ru)-based catalysts exhibited great potential for the alkaline hydrogen evolution reaction. However, the strong adsorption of H on the Ru surface and the undesirable agglomeration of Ru are obstacles to further boosting their hydrogen evolution reaction (HER) performance. Herein, we develop C 60 fullerenol C 60 (OH) 24 to stabilize, disperse, and activate Ru nanoparticles through Ru−O−C 60 connections. Despite the ultrahigh Ru content (38.6 wt %), Ru nanoparticles are densely and uniformly dispersed on the C 60 substrate due to the anchoring and confinement effects of C 60 fullerenols. Moreover, the electron-withdrawing properties of C 60 induce the electrons to flow from Ru to C 60 through the Ru−O−C 60 interface, which enhances the electronic metal−support interaction, thereby optimizing the adsorption behavior of different intermediates. The synthesized Ru−OC 60 -300 has a remarkably small overpotential (4.6 mV at 10 mA cm −2 ) and Tafel slope (24.7 mV dec −1 ), showing high activity and stability toward alkaline HER. Density functional theory simulations reveal that the Ru−O−C 60 interface engineering weakens the Ru−H affinity, promotes water dissociation, and accelerates the hydrogen evolution kinetics.