Pulverization behavior and microstructure evolution with hydrogenation in hydrogen absorbing Ta-Ni intermetallic-based alloys, such as Ta2Ni with Ta solid solution (Tass), TiMn2 with TiMn and Nb3Al with Nb solid solution (Nbss), are investigated to elucidate the mechanism of the hydrogen pulverization. Ta-10at.%Ni consisting of Ta solid solution (Tass) and Ta2Ni Laves phase is pulverized to coarse powder over 100 μm in hydrogenation. Crack propagation occurs preferentially in the brittle Ta2Ni phase rather than in the ductile Tass phase. When the volume fraction of brittle Ta2Ni increases with increasing Ni content, hydrogen pulverization is enhanced. The lattice parameter of Tass increases by hydrogenation, while it does not change in Ta2Ni. In addition, nano-sized regions with Moiré patterns are produced in Tass and Debye rings corresponding to tantalum hydride β-TaH appear in the diffraction pattern. These features are very similar to those of TiMn2 based alloy and Nb3 Al based alloys in the literature. Based on the present results along with those in the literature it is concluded that the hydrogen pulverization is attributable to (1) the absorption of a large amount of hydrogen in constituent phase(s), (2) the large strain introduced by lattice expansion and the hydride formation, and (3) the ease of crack nucleation and propagation in brittle constituent phase(s).