Compounds or complexes with high hydrogen content are viewed as potential hydrogen storage materials. Ammonia borane (NH3BH3, AB in short), with the hydrogen content of 19.6 wt %, is wildly regarded as one of the most promising candidates for hydrogen storage. However, the dehydrogenation of AB occurs at relatively high temperature (100 C and above) with releasing volatile byproducts (NH3 and borazine) and sample foaming. In the previously reports, researchers used mesoporous frameworks or homogeneously catalysis in solution to enhance the dehydrogenation properties. However, the additional weight from the supports or solvents inevitably scarifies the hydrogen density of AB.