The focus of this research is on incorporating and dispersing of niobium particles through the pure magnesium matrix for the means of developing its hydrogen storage performance. For this matter, Nb micro-size particles were embedded between the stacked layers of magnesium foil before implementing accumulative fold-forging (AFF) as a severe plastic deformation (SPD) technique for consolidating a sound layered nanostructured Mg/Nb composite material. Thereafter, the impact of the incorporation of the Nb-particles on the microstructural features and metallurgical bonding between the layers was assessed using advanced microscopy characterizations. As the leading objective, in correlation with the structural development aspects, the hydrogenation and dehydrogenation behaviors of the produced layered nanostructured magnesium-based material associated with the Nb-doping was assessed, with respect to the treated pure magnesium without Nb. The hydrogen storage capacity, charging and discharging temperature, as well as the rate for these storage and release reactions, were obtained as the main properties under investigation and compared with the pure state of magnesium. To this end, the experimental results exhibited an impressive contribution of Nb to improving the kinetics of hydrogenation and dehydrogenation of the nanolayered magnesium structure.