Chemical hydrogen storage involves storing hydrogen in and releasing hydrogen from covalent chemical bonds in molecules and materials. The DOE Center of Excellence for Chemical Hydrogen Storage aims to identify, research, develop, and validate chemical hydrogen storage systems to provide several working options to overcome current barriers and meet 2010 DOE goals for cost-effective, energy efficient, on-board hydrogen storage. The Center comprises seven universities, four companies, and two national laboratories. Researchers in the Center are developing materials and catalysts for hydrogen release and regeneration of spent material spanning a number of integrated projects. Key elements include computation and modeling, the design, synthesis, and testing of structures and compositions to control the thermochemistry and kinetics of hydrogen release and spent fuel regeneration, and engineering assessment of concepts and experimental results. An overview of the Center's objectives and approach will be presented along with a number of results from several different projects.