The development of cost effective catalysts with high activity and 100% selectivity for hydrogen generation from the decomposition of hydrous hydrazine, a promising liquid-phase hydrogen carrier, is a critical challenge for the practical application of hydrous hydrazine to fuel cell vehicles. In this study, noble-metal-free NiCu/CeO2 bimetallic catalysts were readily synthesized using one-step solution combustion synthesis (SCS). The addition of Cu to Ni/CeO2 exhibited a synergistic effect to enhance the catalytic activity for the reaction. Catalyst characterization revealed that the improvement of catalytic performance is attributed to a combination of NiCu alloying, particle size of the active component, and formation of oxygen vacancy in the CeO2 lattice. The tailored 13 wt% Ni0.5Cu0.5/CeO2 catalyst exhibited 100% H-2 selectivity in the temperature range 30-70 degrees C and 3.2-fold higher turnover frequency (TOF) of 1450.0 h(-1) at 50 degrees C as compared to of the Ni/CeO2. This reactivity is also superior to that of most reported non-noble metal catalysts and is even comparable to noble metal-based catalysts.