Philosophiae Doctor - PhD / The main objective of this study was to advance kinetic performances of formation and decomposition of magnesium hydride by design strategies which include high energy ball milling in hydrogen (HRBM), in combination with the introduction of catalytic/dopant additives. In this regard, the transformation of Mg → MgH2 by high energy reactive ball milling in hydrogen atmosphere (HRBM) of Mg with various additives to yield nanostructured composite hydrogen storage materials was studied using in situ pressure-temperature monitoring that allowed to get time-resolved results about hydrogenation behaviour during HRBM. The as-prepared and re-hydrogenated nanocomposites were characterized using XRD, high-resolution SEM and TEM, as well as measurements of the mean particle size. Dehydrogenation performances of the nanocomposites were studied by DSC / TGA and TDS; and the re-hydrogenation behaviour was investigated using Sieverts volumetric technique.