Ni/Al_2O_3 and Ni/xMo-Al_2O_3 catalysts were prepared by impregnation method and the influence of Ni loadings, calcination temperature, the solvents and the additives on catalytic properties of the catalysts was investingated using ammonia decomposition as the model reaction. The catalysts were characterized by XRD and TG-DTG. The results indicated that Ni/Al_2O_3 catalyst exhibited better catalytic activity under the optimum preparation condition of Ni loading 16% (mass fraction), calcination temperature 350℃, and acetone as the solvent. At 500℃ the activity of Ni/Al_2O_3 for ammonia decomposition was significantly increased by 39% by adding 3% Mo to the catalyst and the ammonia conversion of 93.5% was attained over Ni/3% Mo-Al_2O_3 catalyst.