Abstract: Ammonia borane (NH₃BH₃, AB) is considered as an ideal hydrogen storage material for portable hydrogen production. In this paper, a bimetallic carbon cube (Co_0.8Cu_0.2/CNC) catalyst was prepared by high-temperature calcination of the Co_0.8Cu_0.2-ZIF precursor, which was obtained by stirring the reactants at room temperature. In addition, the microstructure and composition of the catalyst were investigated using various characterization methods. The change regularity of the catalyst was explored through the single-variable method. The results showed that the addition of a small amount of Cu had a stabilizing effect on the cubic morphology of the Co_0.8Cu_0.2/CNC catalyst. When the dispersant was CTAB and the calcination temperature was 873 K, the activation energy (E_a) for catalyzing the hydrolysis of AB to hydrogen was 50.79 kJ/mol with the transition frequency (TOF) value as high as 23.37 min⁻¹. Moreover, the catalyst could still catalyze the complete hydrolysis of AB to hydrogen after 25 cycles, which indicated that the catalyst had good stability performance.