Single-atoms (SAs) supported on various substrates have emerged as a new form of electrocatalysts for hydrogen evolution reaction (HER). The exfoliated MXenes possess rich defects/vacancies and surface oxygen groups, can be favorably utilized to anchor SAs. Here, we take advantage of the exfoliated Ti 3 C 2 T x to anchor Ru-SAs on Ti 3 C 2 T x through a wet-chemistry impregnation process. The obtained Ru SA @Ti 3 C 2 T x possesses excellent HER activity, especially under high current densities. Remarkably, Ru SA @Ti 3 C 2 T x can readily attain high current densities of 1 and 1.5 A cm À2 at low over potentials of 425.7 and 464.6 mV, respectively, demonstrating its potential for practical applications. The A 1g vibration frequency shift of the Raman spectrum is innovatively used to probe the surface OH coverage on Ti 3 C 2 T x , providing critical information for mechanistic studies. The experimental and theoretical studies reveal that the superior HER electrocatalytic activity of Ru SA @Ti 3 C 2 T x results from the Ru-SAs enhanced H 2 O adsorption and dissociation, and promoted H 2 formation.