FeTi has one of the highest hydrogen volume storage capacity and its hydride - very favourable absorption/desorption conditions and a high reversibility. However, for applications its low hydrogen mass storage capacity (HMSC) has to be improved. The authors of this paper supposed this would be possible by Al and Ni additions and by a nanocrystalline state. However, FeTi synthesis and alloying with Al and Ni is difficult in a Fe-Ti-Al-Ni system due to the undesired secondary compounds formation. The presented researches proved the possibility of this impediment overcoming and of NiTi-Al-Ni alloy obtaining in a nanocrystalline state, from a mixture of elemental powders of components, by mechano-synthesis carried out in a planetary ball mill, for 24 h, in Ar atmosphere. The obtained alloy proved to have a HMSC of ~3.5 % at 50 0C and 1.5 atm, higher than of FeTi, its dehydrogenation occurring at the same temperature and 1.0 atm.