Hydrogen is expected to be a viable solution for green-energy investment in future. However, hydrogen storage is a big challenge for stationary and mobile applications. Severe Plastic Deformation (SPD) techniques are well-known to be effective in enhancement of hydrogenation in metals hydrides. This paper shows the effect of a novel SPD technique named “High Pressure Torsion Extrusion-HPTE” on the hydrogenation of metal hydrides and compare it with the conventional method of ECAP. Results of mechanical testing and X-ray diffraction patterns showed significant enhancement in hardness and microstructural refinement in materials after HPTE. Accordingly, hydrogenation kinetics improved dramatically. This achievement could be an initiative to implement HPTE in synthesis of metal hydrides for clean energy applications.