We present a model that describes the effect of elastic constraint on the thermodynamics of hydrogen absorption and desorption in biphasic core–shell nanoparticles, where the core is a hydride forming metal. In particular, the change of the hydride formation enthalpy and of the equilibrium pressure for the metal/hydride transformation are described as a function of nanoparticles radius, shell thickness, and elastic properties of both core and shell. To test the model, the hydrogen sorption isotherms of Mg–MgO core–shell nanoparticles, synthesized by inert gas condensation, were measured by means of optical hydrogenography. The model's predictions are in good agreement with the experimentally determined plateau pressure of hydrogen absorption. The features that a core–shell systems should exhibit in view of practical hydrogen storage applications are discussed with reference to the model and the …