Measurements of vibrational excitation and deexcitation of NO (v = 2) scattering from a Au(111) surface show that the probability of both processes increases strongly with the kinetic energy of the incident NO. These results are qualitatively consistent with a vibrational energy transfer mechanism involving electron-hole pairs but not with competing adiabatic models. The form of the energy dependence, and other features of the measurements, are not in accord with existing calculations.