A series of MoO 3 /Al 2 O 3 catalysts with different amounts (molar ratio of CA/Mo = 0, 1, 1.5, and 2) of citric acid (CA) prepared by simultaneous impregnation were evaluated for sulfur-resistant methanation. Based on the evaluation results, catalytic activity increased accompanied with the rise of citric acid amount. Combine with the analysis of N 2 -physisorption, XRD, H 2 -TPR, XPS, and TEM, the catalyst saturated loading capacity improved, resulting in increasing dispersion of Mo species on Al 2 O 3 surface clearly. According to H 2 -TPR result, the Mo oxide precursors can be more easily sulfureted when citric acid is added. Moreover, based on the Raman analysis, increasingly tetrahedrally coordinated Mo 6+ species with high methanation performance are generated after citric acid treatment. These factors probably together accelerate MoO 3 /Al 2 O 3 catalytic activity growth for methanation.