In this paper, a three-dimensional hydrogen absorption model is developed to precisely study hydrogen absorption reaction and resultant heat and mass transport phenomena in metal hydride hydrogen storage vessels. The 3D model is first experimentally validated against the temperature evolution data available in the literature. In addition to model validation, the detailed simulation results shows that at the initial absorption stage, the vessel temperature and H/M ratio distributions are uniform throughout the entire vessel, indicating that the hydrogen absorption is so efficient during the early hydriding process and thus local cooling effect is not influential. On the other hand, nonuniform distributions are predicted at the latter absorption stage, which is mainly due to different degrees of cooling between the vessel wall and core regions. This numerical study provides the fundamental understanding of detailed heat and mass transfer phenomena during hydrogen absorption process and further indicates that efficient design of storage vessel and cooling system is critical to achieve fast hydrogen charging and high hydrogen storage efficiency.