MXene, a family of 2D transition metal carbides and nitrides, presents promising applications in electrocatalysis. Maximizing its large surface area is key to developing efficient non-noble-metal catalysts for the hydrogen evolution reaction (HER). In this study, oxygen-functionalized Ti₃C₂T_x MXene (Ti₃C₂O_x) is synthesized and deposited gold nanoparticles (Au NPs) onto it, forming a novel composite material, Au-Ti₃C₂O_x. By selectively removing other functional groups, mainly -O functional groups are retained on the surface, directing electron transfer from Au NPs to MXene due to electronic metal-support interaction (EMSI), thereby improving the catalytic activity of the MXene surface. Additionally, the interaction between Au NPs and -O functional groups further enhanced the overall catalytic activity, achieving an overpotential of 62 mV and a Tafel slope of 40.1 mV dec⁻¹ at a current density of −10 mA cm⁻² in 0.5 m H₂SO₄ solution. Density functional theory calculations and scanning electrochemical microscopy with ≤150 nm resolution confirmed the enhanced catalytic efficiency due to the specific interaction between Au NPs and Ti₃C₂O_x. This work provides a surface modification strategy to fully utilize the MXene surface and enhance the overall catalytic activity of MXene-based catalysts.