Crystalline Pd 1− x Ag x –H y ( x = 0 – 0.35 ) alloys were studied as model systems representing a chemically disordered system for hydrogen-storage materials. Extensive H 1 relaxation rate ( R 1 , R 1 ρ and R 2 ) measurements were carried out in a wide temperature range of 2.4–400 K. Palladium–silver alloys of silver concentration as high as 35 at.% were studied by NMR spectroscopy for the first time. The relaxation mechanisms magnetic dipolar relaxation (hydrogen diffusion), Korringa relaxation, relaxation by paramagnetic impurity ions and cross-relaxation to quadrupolar metal nuclei were identified and characterized. The presence of cross-relaxation between H 1 and quadrupolar Pd 105 nuclear spins was assumed and demonstrated for the first time in Pd–H and Pd 1− x Ag x –H systems. More than one jump processes of diffusing hydrogen were found to be present in the studied palladium–silver alloys. Only lower estimated limit values of Korringa constants could be obtained since no frequency independent R 1 versus T region was found. These values are significantly higher than the ones reported by others.