Two-dimensional (2D) carbide and nitride MXenes possess properties that are desirable for a broad range of electrocatalytic applications including the hydrogen evolution reaction (HER). These properties include high surface area, hydrophilicity, heterogeneity of redox-active transition metals, and tunable surface functionalities allowing for low HER overpotentials. In this paper, we report on the cathodic etching and À O/À OH functionalization of hybrid Ti 3 CN upon the application of an external potential for improved HER performance and show that the active sites for HER on this MXene catalyst are located primarily on the À OÀ and À OH functional groups. The overpotential for the hybrid Ti 3 CN improves by 350 mV upon in-situ À O/À OH functionalization and etching, reaching À 0.46 V vs. RHE at a current density of 10 mA cm À 2 , much lower than those reported for the benchmark Ti 3 C 2 carbide MXene. These results provide a path forward to tuning the electrocatalytic activity of MXenes and related electrocatalysts for water splitting.