SignificanceSurfaces are gates to control the transport of energy and materials between the gas phase and bulk. For the hydrogen storage, the transport of hydrogen across the surface is recognized as the bottleneck, e.g., 1 H2 in 1,000 impinging a Pd surface penetrates the surface. Here, we demonstrate that alloying the Pd(110) surface with submonolayer amounts of Au dramatically accelerates the hydrogen absorption, by a factor of more than 40. This discovery will lead to enhancement of hydrogen absorption kinetics, thereby improving the performance of hydrogen-purifying membranes and hydrogen-storage materials, which is a key for utilizing hydrogen as a carbon-free energy carrier.