Efforts to thermodynamically destabilize magnesium hydride (MgH2), so that it can be used for practical hydrogen storage applications, have been a difficult challenge that has eluded scientists for decades. This letter reports that MgH2 can indeed be destabilized by forming solid solution alloys of magnesium with group III and IVB elements, such as indium. Results of this research showed that the equilibrium hydrogen pressure of a Mg-0.1In alloy is 70% higher than that of pure MgH2. The temperature at 1 bar hydrogen pressure (T1bar) of Mg-0.1In alloy was reduced to 262.9 °C from 278.9 °C, which is the T1bar of pure MgH2. Furthermore, the kinetic rates of dehydrogenation of Mg-0.1In alloy hydride doped with a titanium intermetallic (TiMn2) catalyst were also significantly improved compared with those of MgH2.