A comparative study of Mg 5.7 In 0.3 Ag and Mg 6 Ag alloys was conducted to reveal the effects of indium (In) solid solutions on the hydrogen storage properties of Mg-based alloys. Different from the Mg 6 Ag alloy, the as-cast Mg 5.7 In 0.3 Ag alloy was composed of a Mg(In) solid solution and Mg 3 Ag. However, an initial hydrogen absorption/desorption treatment (i.e., activation) propelled the In atoms in Mg(In) toward Mg 3 Ag, forming (Mg, In) 3 Ag in the activated sample. This transformation involving the dissolution of In atoms from Mg into solid Mg 3 Ag not only greatly improved the thermodynamics of hydrogen desorption but also enhanced its catalytic effect on hydrogen desorption from additional MgH 2 . The (Mg, In) 3 Ag-H 2 system exhibited altered thermodynamics, as its enthalpy change of the hydrogen desorption was 62.6 kJ mol À1 H 2 . Moreover, the activation energy of the hydrogen desorption from the Mg 5.7 In 0.3 Ag sample was lowered to 78.2 kJ mol À1 .