Hydrous hydrazine (N2H4∙H2O) has been considered a promising chemical hydrogen storage carrier compound due to its high hydrogen content and easy recharge as a stable liquid for transportation. NiPt, CoPt, and CoNi nanoparticles (NPs) supported on Al(OH)3 Nano sheets are prepared in this research for hydrogen production by N2H4∙H2O catalytic decomposition. Experimental results indicated that the prepared NiPt, CoNi, and CoPt NPs have superior catalytic efficiency than that of published catalysts for the N2H4∙H2O dehydrogenation. It approximately released 3 Equiv. (H2 + N2) corresponding with TOF values of 1280, 359, and 342 hours−1 at 298 K, respectively. Prepared NiPt-Al(OH)3 and CoPt-Al(OH)3 possess good paramagnetic characteristics and can be easy to separate and reuse by a magnet. Meanwhile, prepared catalysts also perform good recyclability and approximately 100% selectivity after five durability tests. The crystallinity and amorphous phase percentage of NiPt-Al(OH)3, CoNi/Al(OH)3, and CoPt/Al(OH)3 were ranged from 4.29% to 15.18% and from 84.82% to 95.72%, respectively. The catalytic performance of these above catalysts can be recognized by the electronic interaction between the Al(OH)3 Nano sheet and Ni, Co, and Pt NPs. Meanwhile, the Al(OH)3 Nano sheet surface could provide strong basic active sites with corresponding synergistic cooperative influences between ultra-fine monometallic and bimetallic NPs and Al(OH)3 Nano sheets. In summary, the prepared Ni, Co, and Pt-based catalysts have been developed for the application of N2H2∙H2O dehydrogenation as a favorable hydrogen storage material.