Before hydrogen can find widespread use as a fuel, significant challenges associated with producing and reversibly storing hydrogen must be overcome. Accurate computational methods can play an important role in accelerating efforts to develop robust materials for these two tasks. I will describe how first principles calculations have been used to screen candidate materials for hydrogen separation using metal alloy membranes and for reversible hydrogen storage using destabilized metal alloys. The results of these calculations identify important topics for continuing theoretical and experimental efforts.