The original and high-pressure torsion (HPT) processed Zircaloy-4 materials were hydrided using gaseous hydrogen charging at different hydrogen pressures (10, 15 and 20 atm). The phase and microstructural evolutions of the samples during hydriding were characterized. It showed that when hydriding at the identical conditions, more hydrides tended to form in the HPT samples compared to that of the original ones. At a hydrogen pressure of 20 atm, the HPT sample was completely converted to ε-ZrH2 while some δ-ZrH1.66 hydrides (volume fraction ~5.73%) were present in the material without HPT preprocessing. The HPT samples exhibited high potential for the hydride precipitation, and the large concentration of lattice defects induced by HPT was considered to be responsible for this enhanced susceptibility.