The vibrational spectra of hydrogen and parameters of H diffusion in the coarse-grained C15-type system ZrCr(2)H(3) and in nanostructured ZrCr(2)H(3) have been studied by means of inelastic and quasielastic neutron scattering. It is found that the diffusive motion of hydrogen in coarse-grained ZrCr(2)H(3) can be described in terms of at least two jump processes: a fast localized H motion with the jump rate τ(l)( - 1) over the hexagons formed by interstitial Zr(2)Cr(2) sites and a slower process with the rate τ(d)( - 1) associated with H jumps leading to long-range diffusion. While τ(d)( - 1)(T) in the range 250-380 K follows the Arrhenius law with the activation energy of 142 ± 4 meV, the temperature dependence of τ(l)( - 1) deviates from Arrhenius behavior. The nanostructured ZrCr(2)H(3) samples prepared by ball milling consist of C15-type grains and strongly distorted (amorphous-like) regions. H atoms in the strongly distorted regions are found to be immobile on the time scale of our experiments. The microscopic picture of H jump motion in the C15-type grains of the nanostructured samples is similar to that in coarse-grained ZrCr(2)H(3); however, the ball milling leads to a considerable decrease in the jump rate τ(d)( - 1).