The recyclable dehydrogenation of ammonia borane (AB) is achievable within a graphene oxide (GO)-based hybrid nanostructure, in which a combined modification strategy of acid activation and nanoconfinement by GO allows AB to release more than 2 equiv of pure H-2 at temperatures below 100 degrees C. This process yields polyborazylene (PB) as a single product and, thus, promotes the chemical regeneration of AB via reaction of PB with hydrazine in liquid ammonia.