This report summarizes the 5-year R&D activities within the U.S. Department of Energy Metal Hydride Center of Excellence (MHCoE). The purpose of the MHCoE was to conduct highly collaborative and multi-disciplinary applied R&D to develop new reversible hydrogen storage materials for light-duty vehicles. The MHCoE combined three broad areas: (a) mechanisms and modeling, which provided a theoretically driven basis for pursuing new materials, (b) materials development, in which new materials were synthesized and characterized and (c) system design and materials engineering, which provided the foundational information to enable new materials to be realized as practical automotive hydrogen storage systems. The MHCoE was organized into four materials-oriented "projects," along with one engineering project. Results from all of the projects are given, as well as an account of the downselection process that identified materials to be pursued further after initial investigation. The downselected materials are compared against material goals derived from the revised 2010 DOE hydrogen storage system targets for light-duty vehicles. Suggestions and recommendations for further R&D directions are given, based on the MHCoE findings. Copyright (C) 2013, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.