Kaolin as a raw material for mesoporous support was firstly modified by calcination, acid treatment, and then was used to prepare nickel catalysts. The amount of alumina which was activated in kaolin during thermal treat-ment and then leached out in the acid was different. XRD patt of the kaolin calcined at 600 °C or 900 °C exhib-ited only the diffraction peaks for amorphous silica and quartz while that calcined at 1100 °C showed obvious peaks forγ-Al2O3. Therefore, the nickel-based catalysts exhibited different physic-chemical properties. Atmo-spheric syngas methanation over the catalysts clarified an activity order of CA-1100>CA-900>CA-1400>CA-600>KA≈0 at temperatures of 350–650 °C and a space velocity of 120 L·g?1·h?1. Metallic nickel with small diameter which has medium interaction with the modified kaolin and is well dispersed on the support would have reasonably good activity and carbon-resistance for syngas methanation.