Bimetallic Ni1Cu8/γ‐Al2O3 catalysts were prepared by using atomic layer deposition (ALD) and impregnation methods. By combing N2 adsorption/desorption, N2O oxidation followed by H2 titration, X‐ray diffraction (XRD), transmission electron microscopy (TEM), and temperature‐programmed reduction (TPR), we showed the differences in the physicochemical properties of the bimetallic catalysts between the two methods. The results indicated that the sample prepared by the ALD method has a higher CH3OH yield (1.5 mmol g−1 h−1) than the sample obtained by the impregnation method (0.7 mmol g−1 h−1). The highly dispersed alloy particles and stronger interaction between Cu and Ni are the key factors for the enhanced catalytic performance of the sample prepared by the ALD method.