Nickel and platinum were used to prepare a series of core@shell structures to be studied as catalysts for the dehydrogenation of aqueous hydrazine borane N2H4BH3 at 50 °C. The challenge was especially to get a maximum of 3 mol of gas by decomposition of the N2H4 moiety. In our conditions, the most efficient Ni@Pt was found to be the structure constituted of 5 atoms of nickel for 1 atom of platinum. This catalyst permits to generate up to 4.5 mol H2 + N2. Surface characterizations showed that the efficiency of this catalyst is due to the presence of both metals on the surface, suggesting therefore that the structure would be rather Ni@NiPt. Our main results are reported herein.