Hydrogen as a fuel has the potential to reduce fossil fuel dependence while reducing environmental emissions; however, adoption of a hydrogen economy will require significant developments in infrastructure, synthesis, distribution, and hydrogen storage. For storage, the DOE has set stringent targets based on scientific (e.g. energy density, delivery temperature, desorption rates) and practical considerations (e.g. system cost, safety considerations, release). No one currently available storage technology meets all targets. The current work will discuss the reliability of hydrogen uptake methodology, limitations and promise of existing materials, and the development of composite materials for hydrogen storage. Particular emphasis will be placed on design of materials through: the synergistic hydrogen spillover effect in composites, the use of chemical modeling for informed material selection, the introduction of low-cost natural materials, and controlled selection of pretreatment and synthesis parameters to impart certain hydrogen storage characteristics.