The mechanically alloyed amorphous alloys of the Tisub.45Zrsub.38Nisub.17 composition are known for their ability to form a quasicrystalline state after thermal treatment. It is also known that the amorphous and quasicrystal alloys belonging to the Tisub.45Zrsub.38Nisub.17 family are able to store hydrogen and yield gravimetric densities above 2 wt.%. In this contribution, we report the results of research on the Tisub.45Zrsub.38Nisub.17 system with vanadium doped instead of titanium. We found that the amorphous samples with moderate doping (x < 20) show the ability to absorb hydrogen while maintaining the amorphous state and they transform into the novel glassy-quasicrystal phase during annealing. Those materials with higher vanadium concentrations do not form entirely amorphous structures. However, they still can absorb hydrogen easily. It was also confirmed that the in situ hydrogenation of the amorphous alloys is a straightforward process without decomposition of the alloy. In this process, hydrogen does not attach to any particular constituent of the alloy, which would lead to the formation of simple hydrides or nanoclusters. Therefore, we were able to confirm the fully amorphous nature of the deuterides/hydrides of the Tisub.45−xVsub.xZrsub.38Nisub.17 with moderate V doping.