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AB5-based hydrogen storage thin films (LaNi4.25Al0.75), deposited on Cu substrate by dc magnetron sputtering were investigated in this study. X-ray diffraction (XRD) revealed that the microstructure of the layer was in crystal form. SEM and AFM analyses proved that the film appeared to be rather rough with numerous randomly sized pores of approximately 15-40 in nm diameter. Structural stability of the film was examined by the combined analyses of DSC, XRD, and SEM, which indicated that this film maintained its structural stability below 500 K or so, and a network structure was ob served on the film after being heated at 700 K for 30 min. Electrochemical hydrogen-storage properties of the films were investigated by simulated battery tests. It was found that single-layered LaNi4.25Al0.75 film exhibited electrochemical hydrogen-storage properties similar to typical AB5 alloys in bulk, and the maximum discharge capacity of the film was about 220 mAh/g. After 20 charge/discharge cycles, small needle-shaped aluminium oxide was formed on some fractions of the film surface.