The phase structure and hydrogenation behavior of the (Sr1-xCax)(2)Al (x = 0.5, 0.6, 0.7, 0.8 and 0.9) alloys were investigated. It was found that the (Sr1-xCax)(2)Al alloys have different phase components with the change of Ca content. When x = 0.6 and 0.7, the single (Sr, Ca)(2)Al phase can be obtained. The lattice parameters of (Sr, Ca)(2)Al compound in the (Sr1-xCax)(2)Al alloys decrease gradually with the increase of Ca content. The (Sr, Ca)(2)Al phase can absorb hydrogen even at 303 K. During hydrogenation, the (Sr, Ca)(2)Al compound transforms into distinct phases at different temperatures. (c) 2008 International Association for Hydrogen Energy. Published by Elsevier Ltd. All rights reserved.