Every energy-related application of hydrogen requires its safe and efficient storage, especially in transportation where there are severe weight and volume constraints. Hydrogen fuel can be stored as a compressed gas, a cryogenic liquid, or in a hydrogen-rich solid. The first two approaches necessitate substantial energy for compression or liquefaction, and therefore, entail multiple containment and safety issues. Conversely, hydrogen-rich solids remain the safest media to store, deliver and distribute high-purity hydrogen required for automotive fuel cells and, as an added benefit, assure exceptionally high volumetric density of the fuel. Although large scale commercial applications of hydrogen in transportation may be several decades away, real progress in ultra-high capacity hydrogen storage materials, which has been truly the bottleneck in hydrogen-based distributed energy, is required now. One of the promising compounds is lithium tetrahydroaluminate – LiAlH4 – containing a total of 10.5 per cent hydrogen by weight, half of which is available at room temperature and a quarter below ~150ºC, thus making it a nearly 8 wt.% H2 material. Chemical transformations induced by mechanical energy are effective in dehydrogenation of LiAlH4 and in solid state synthesis of hydroaluminates, and therefore, mechanochemistry is a feasible pathway towards the reversible hydrogen storage in complex hydrides.