The laser engineered net shaping technique was applied as a fast synthesis method for preparing libraries of binary and ternary alloys. Compositional gradient libraries of Fe-Ti alloys and four different FeTiNi samples were fabricated from elemental powders. A continuous gradient sample and discrete gradient samples (25 and 188 samples) were deposited. Ternary alloys were prepared from pre-blended powder mixtures. Chemical composition measurements showed that samples of different compositions can be synthesized. XRD phase analysis indicated that structures close to equilibrium or occasionally quenched are obtained after the process. The microstructure of the prepared samples was analyzed. The hydrogen storage properties of the selected samples were investigated. After laser deposition, the samples were found to absorb significant quantities of hydrogen with just a simple activation. The method was determined to be very useful for discovering new ternary and multicomponent alloys for hydrogen storage. Copyright (C) 2013, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.