The times of nuclear spin–lattice relaxation have been measured and the spectra of NMR for 1H and 27Al in Ti3AlHx hydrogenated intermetallic compounds with hydrogen concentrations of х = 0, 0.31, 0.51, 1.0, 2.0, and 4.32 in a wide range of temperatures (10–500 K) and resonance frequencies (8.2–90 MHz) have been recorded. The analysis of low-temperature relaxation data has shown that the addition of hydrogen with a concentration of х ≥ 2 leads to a significant change in the density of electron states at the Fermi level. It has been found that the hydrogen mobility in Ti3AlHx strongly depends on its concentration. For solid solutions of hydrogen in Ti3Al with х < 1, the mobility of hydrogen atoms on the scale of frequencies of NMR in the investigated temperature range has not been detected. In Ti3AlHx compounds with х ≥ 2, the fast diffusion of hydrogen is observed, which can be related to changes in the structure of these compounds.