2 (g) + 2H 2 (g)). [4] This corresponds to a theoretical gravimetric hydrogen storage capacity of 10.0 wt% for the HB-3H 2 O system, which is much higher than those of NaBH 4 -4H 2 O (7.3 wt%), NH 3 BH 3 -4H 2 O (5.9 wt%), and N 2 H 4 ·H 2 O (8.0 wt%). [5] However, in order to maximize the efficiency of N 2 H 4 BH 3 as hydrogen storage materials, the incomplete and undesired decomposition (3N 2 H 4 → 4NH 3 (g) + N 2 (g)) to ammonia (NH 3 ) must be avoided, because ammonia is toxic to fuel cell catalysts. [6] It has been reported that monometallic nanoparticles (NPs), such as Ni, Ru, and Pd, are only effective in hydrolyzing BH 3 group in HB as N 2 H 4 moiety does not participate, corresponding to a conversion of 50%. [7] Recently, some noble-metal-containing (e.g., Pt, Rh, and Pd) Ni-based heterogeneous catalysts have been developed as catalysts for high-extent dehydrogenation of HB, although the conversion and activity has been improved, the limited resources and expensive cost of noble metal still hinder their practical applications. [8] Therefore, from the viewpoint of practical application, the development of low-cost and high-efficient noble-metal-free catalysts to further improve the catalytic activity, selectivity, and conversion rate under moderate conditions is the key to realize safe and efficient hydrogen storage, thus could provide more possibilities to enter H 2 economy society. Boron nitride (BN), a material analogous to the structure of graphite, has been considered as a promising catalyst support owing to its high chemical stability, nontoxicity, and large surface area. [9] Herein, we first report a facile methodology for synthesizing BN-supported noble-metal-free Ni-MoO x /BN nanocatalyst without the help of a surfactant by a sequential impregnationreduction approach. Unexpectedly, the resultant Ni-MoO x /BN leads to the 100% conversion, 100% H 2 selectivity, and superior catalytic activity toward the dehydrogenation of HB in an alkaline solution at 323 K, with a turnover frequency (TOF) value of 600.0 h −1 , which is even better than most of the noble metal heterogeneous catalysts. [8,10] Ni-MoO x /BN composite is synthesized by a wet-chemical method as illustrated in Scheme 1. First, BN (15 mg) is dispersed in H 2 O (5 mL) through sonicating treatment. Subsequently, NiCl 2 ·6H 2 O (0.1 m, 1 mL) and Na 2 MoO 4 ·2H 2 O (0.1 m, 1 mL) aqueous solutions are impregnated to the BN Hydrazine borane (HB) has been considered as a promising hydrogen storage material due to its high hydrogen content and stability at room temperature. For the first time, a facile wet-chemical method is developed to synthesize amorphous/low crystalline noble-metal-free Ni-MoO x /BN composite as a lowcost and high-efficient catalyst for hydrogen generation from HB decomposition. The as-prepared Ni-MoO x /BN hybrid exerts 100% selective conversion and can catalyze HB complete decomposition within 5 min, corresponding to a turnover frequency (TOF) value of 600.0 h −1 at 323 K. The excellent catalytic activity may be attribut...