The hydrogenation characteristics of the sputtered Ti-Mo (alpha-beta alloy) films (similar to 900 nm) with and without Ni coating were investigated using high-energy non-Rutherford backscattering (non-RBS) and elastic recoil detection techniques. It was found that the Ti-Mo alloy had a good hydrogen absorption capability compared with pure Ti, and showed a high resistance to C contamination as well. It was also demonstrated that with a top layer of thin Ni film on the Ti-Mo, an improvement in hydrogenation capability was achieved. The non-RES spectra revealed that the Ni layer reduced the surface contamination of C and O impurities effectively and, therefore, promoted hydrogen absorption activation. On the other hand, there was little change in their maximum hydrogen storage capability with increasing Mo concentration (Mo <20 at. %), and the phases in the samples hydrogenated at 473 K were composed of a hydride and a beta -solid solution. Once the Mo content approached 20 at. %, the delta phase disappeared and only the beta phase existed in the film. The durability of the sputtered films on the Mo substrate against the hydrogen absorption/desorption was also measured with the hydrogen absorption-desorption cycles method, and a significant improvement was obtained.