Hydrogenation under high pressures up to 3 GPa and at elevated temperatures up to 393 K was used to introduce structural changes in the bulk and on the surface of Cu-Zr amorphous alloys which then were examined by XRD and microscopy. The hydrogenative pre-treatment at a high hydrogen fugacity followed by annealing at 623 K, aimed at desorption of hydrogen, and an eventual exposure of the samples to air at room temperature to oxidize Zr, resulted in a distinct increase of catalytic activity in the dehydrogenation of 2-propanol. A tentative mechanism to account for enhancing the catalytic activity induced by the above combined pre-treatment including correlations between catalytic performance (activity, selectivity) and physical characteristics (morphology, XRD features, Cu(0) specific surface areas) is discussed.