Three-layered Pd/Mg1-x Al (x) /Pd (x = 0, 0.13, 0.21, 0.39) thin films were prepared by means of pulsed laser deposition. In the present Al concentration range, X-ray diffraction analyses showed that the Mg1-x Al (x) layer was constituted of a single phase Mg(Al) solid solution. The Mg(Al) grains are preferentially orientated along the c-axis and their size decreased (from 18.5 to 10.5 nm) as the Al content increased. Scanning electron microscopy and atomic force microscopy observations indicated that all the films exhibited a globular surface structure. However, the surface roughness of the films decreased as the Al concentration increased. Rutherford backscattering spectroscopy revealed that the Mg-Al layer density (porosity) was strongly dependent on the Al content. Successive hydriding charge/discharge cycles were performed on the different Pd/Mg1-x Al-x/Pd films in alkaline media. The highest discharge capacity was obtained with the Pd/Mg0.79Al0.21/Pd film, namely similar to 85 mu Ah cm(-2) mu m(-1) or 320 mAh g(-1), which corresponds to a H/M atomic ratio of similar to 0.48 in the Mg-Al layer.