For reversible hydrogen storage properties of 17MgH 2 + 12Al § Mg 17 Al 12 + 17H 2 , MgH 2 /Al nanocomposites (I)(IV) synthesized by ball milling of MgH 2 and Al (or AlH 3 ) were studied in connection with milling conditions. The milling processes consisting of two steps were effective to improve the hydrogen storage behavior; MgH 2 was first milled with solutions of triethylaluminium (TEA) in hexane, followed by addition of Al and TEA solutions. The mixtures were further milled to yield the nanocomposite (III). In preparing the nanocomposite (IV), AlH 3 was used instead of Al. For the nanocomposites (III) and (IV), it was proved by XRD, TDS, DSC and PCI that such ball-milling led to high dispersion of nanocrystalline MgH 2 in Al and/or AlH 3 matrix in the resulting nanocomposites. In DSC measured under a 0.1 MPa hydrogen atmosphere, the nanocomposites (III) and (IV) exhibited reversible H 2 absorption and desorption at 493503 and 573593 K, respectively.