This article presents an investigation into the impact of High Pressure Torsion Extrusion (HPTE) on the microstructural features, hardness and hydrogen storage, focusing on pure magnesium. HPTE is a modern mechanical nanostructuring technique that can refine the microstructural properties and subsequently affects the mechanical and functional properties of the materials. Two HPTE regimes were used in this study: (1) Direct Extrusion without rotation (DE), and (2) an extrusion speed of 6 mm/min along with a rotational speed of 1.8 rpm (v6w1.8). One sample in as-received conditions was also tested as a reference. Results showed increased hardness in the material after HPTE processing, with the DE sample reaching 60 HRB and the v6w1.8 sample exhibiting a gradient distribution of hardness from 71 to 83 HRB. X-ray diffraction analysis revealed significant microstructural refinement in the v6w1.8 sample. Results of hydrogenation kinetics showed that the DE sample absorbed up to 1.2 wt.% of hydrogen, while the v6w1.8 sample displayed 7.2 wt.% of hydrogen absorption, approaching the theoretical hydrogen storage capacity for magnesium (7.6 wt.%). These findings highlight the positive effects of HPTE on microstructural refinement and hydrogen storage, showcasing its potential for advancements in materials science and hydrogen-based energy technologies.