Amorphous and nanocrystalline Mg-based alloys (Mg65Cu25)100-xNdx (x=2,5,7,10) were prepared by melt-spinning. The microstructure of the as-quenched ribbons was characterized and the hydriding properties of these alloys were measured. The experiment results show that the as-quenched amorphous (Mg65Cu25)93Nd7 alloy display the best hydriding properties (hydriding kinetics and hydrogen absorption capacity),its maximum hydrogen capacity is 3.0 wt%H. The nanocrystalline (Mg65Cu25)98Nd2 alloy shows slower hydriding kinetics and lower hydrogen absorption capacity compared to the other Mg-Cu-Nd amorphous alloys. It is conformed that the glass-forming ability becomes strong with the increase of neodymium for the as-quenched (Mg65Cu25)100-xNdx alloys,which leads to the high H-capacity.