Three-layered Pd/Mg/Pd thin films were prepared by pulsed laser deposition in the presence of helium gas. For Pd layer deposition, the He pressure was fixed at 200 mTorr whereas different pressures of He were used for Mg layer deposition (50, 200 and 600 mTorr). The degree of crystallinity and of (001) texture in the Mg layer increase with increasing He pressure. In addition, the increase in He pressure upon Mg deposition greatly accentuates the roughness of the Mg layer, which induces an extension of the outer Pd/Mg interface region. In contrast, the inner Pd/Mg interface is sharp for all the Pd/Mg/Pd films. The electrochemical hydrogen sorption properties of the Pd/Mg/Pd films are improved by increasing the He pressure for Mg layer deposition. However, the maximum H-solubility in the Mg layer remains low (H/Mg similar to 0.26) and is not significantly increased by the presence of the inner Pd layer, indicating that Mg hydride phase is confined in the outer Pd/Mg interface region. (C) 2009 International Association for Hydrogen Energy. Published by Elsevier Ltd. All rights reserved.