Ni-Al 2 O 3 catalysts prepared by solution combustion method for syngas methanation were enhanced by employing various heating rate and different solvent. The catalytic properties were tested in syngas methanation. The result indicates that both of heating rate and solvent remarkably affect Ni particle size, which is a key factor to the catalytic activity of Ni-Al 2 O 3 catalysts for syngas methanation. Moreover, the relationship between Ni particle size and the production rate of methane per unit mass was correlated. The optimal Ni-Al 2 O 3 catalyst prepared in ethanol at 2°C/min, achieves a maximum production rate of methane at the mean size of 20.8 nm.