Recently calcium hydride has attracted attention as a possible component in ternary complex hydrides such as Ca(AlH4)(2), Ca2SiHx and quaternary complex hydrides of the type Li-B-Ca-H. Although in bulk form CaH2 decomposes reversibly above 600 degrees centigrade we were motivated to see whether calcium hydride in cluster form has properties suitable for hydrogen storage. We report here the results of DFT calculations using VASP (R) package for clusters CanH2n with n = 1, 2, 3, 4, 6, 8, 10, 12, 14, 16, 20 to get the ground state geometries, energies, bond lengths, and desorption energies, after molecular dynamics optimization. The desorption energy vs. cluster size n curve showed that the desorption energy goes up sharply to similar to 1.4 eV per H-2 for n up to 4, followed by a broad maximum of similar to 1.8 eV per H-2 around n = 12-14, and then tapers off to a nearly constant value of 1.6 eV per H-2 approximating bulk behavior, which compares favorably with previously reported results. Comparison of these results with those of MgnH2n shows that CanH2n has a lesser potential as a hydrogen storage medium. Copyright (C) 2011, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.