The technological applications of MgH2 hydrides for hydrogen storage demand the overcoming of some critical issues: an improvement of the reaction kinetics and a reduction of the desorption temperature. The synthesis of nanocrystalline MgH2 by reactive milling and inert gas condensation and a proper metal catalyst addition, constitute recently employed strategies. In the investigation of the hydrogen short and long-range dynamics, sorption kinetics and nanostructure stability, the mechanical spectroscopy offers some specific advantages. In the present research this technique was employed with other experimental approaches (XRD DSC) to investigate relaxational and structural damping processes in nanocrystalline MgH2 with added catalysts (Fe). Time/temperature variation of the dynamic elasticity moduli and mechanical quality factor are correlated to hydrogen anelastic relaxation processes and concomitant structural transformation of MgH 2 to Mg associated to long range H diffusion. Results are discussed with reference to microstructural modification strategies able to assist hydrogen release.