We describe a new hydrogen storage platform based on well-defined BN heterocyle materials. Specifically, we demonstrate that regeneration of the spent fuel back to the charged fuel can be accomplished using molecular H(2) and H(-)/H(+) sources. Crystallographic characterization of intermediates along the regeneration pathway confirms our structural assignments and reveals unique bonding changes associated with increasing hydrogen content on boron and nitrogen. Synthetic access to the fully charged BN cyclohexane fuels will now enable investigations of these materials in hydrogen desorption studies.