Achieving the "on-off" control of hydrogen release remains a huge challenge in efficiently harnessing hydrogen energy on demand. In this work, a controlled hydrogen production strategy is proposed. Hydrogen carrier ammonia borane (AB) and Co catalyst are loaded into kaolinite aerogel (KA) to obtain a composite AB@Co/KA monolith. The results show that Co particles with surface-oxidized species are uniformly decorated on the surface of aerogel, and AB can fill the pores of aerogel to form a composite hydrogen storage material. Hydrogen generation is modulated on AB@Co/KA by tuning the amount of water added, which achieves an "on-off" hydrogen release on demand. The Co-modified KA (Co/KA) can be repackaged multiple times for recycling use after the AB is completely hydrolyzed. This work provides a promising approach for controlling the release of hydrogen neither the input of additional energy nor foreign reagents added to the reaction system.