Hydrogen‐storage materials (HSMs) have especially revolutionized the field of “hydrogen storage” by offering a relatively safe storage alternative and high gravimetric hydrogen density. However, a critical challenge is storage reversibility. This is the central tenet of the present article, which discusses ways to close the hydrogen cycle with solid‐ and liquid‐phase HSMs. A distinction between the different HSMs is made on the basis of the approach under which they can be rehydrogenated; this led to the proposition of distribution in three categories: one, materials allowing reversible storage of H2; two, hydrogen carriers for which the byproducts must be recycled; three, sustainable hydrogen carriers with which the hydrogen cycle is considered as being byproduct free. From our analysis, supported by many examples, it seems that the hydrogen cycle can be closed with all of the HSMs discussed herein and that the dehydrogenation/rehydrogenation paths depend on their nature.