Both static and magic-angle spinning ͑MAS͒ 2 H nuclear magnetic resonance spectroscopy indicate that two inequivalent sites are occupied in ZrNiD 3.0 , in a 2:1 ratio, in agreement with previous work. The sites occupied in the trihydride phase have been previously identified as Zr 3 Ni and Zr 3 Ni 2 . In ZrNiD 1.0 , two well-resolved lines of equal intensity are observed in the MAS spectrum at temperaturesϽ220 K, indicating that two other inequivalent sites are occupied in a 1:1 ratio, in contrast with previous reports that only one type of site (Zr 4 Ni 2 ) is occupied in the monohydride ͑͒ phase at room temperature and above. The temperature dependences of both MAS and static ZrNiD 1.0 spectra indicate that no phase transitions occur over the entire temperature range studied, 160-500 K. The deuterium hopping rate in ZrNiD 1.0 is determined from characteristic changes in the MAS spectra as a function of temperature; the motion is consistent with an activation energy E a Х0.44 eV assuming a rate prefactor 1/ 0 ϳ10 13 s Ϫ1 . In ZrNiD 3.0 , the rate of deuterium motion is determined from signatures of motion in the static and MAS spectra. The motion in ZrNiD 3.0 is consistent with an activation energy E a Х0.62 eV assuming a rate prefactor of ϳ10 13 s Ϫ1 .