The collisional thermalization of hot H atoms produced by the excimer laser photolysis of H2S (193 nm) and HI (193 and 248 nm) has been determined by measuring the decrease in vibrational excitation of CO2 (ν3) as a function of moderator pressure. Cross sections obtained for the rare gases in this way are in reasonable agreement with those calculated for energy loss in hard-sphere collisions. These experiments also indicate that the efficiency of vibrational excitation increases as the relative translational energy increases.