By a post synthesis method, nickel (Ni) particles could be grafted onto SBA-15 for the first time through a chemical bond (-O-Ni-O-Si-O-) formation between silicon (Si) and Ni via oxygen (O) using Ni ammonia (NH3) complex ions (Ni(NH3)x) 2+ with NH3/Ni mole ratio of 1~5, which existed as Ni phyllosilicate on SBA-15 surface, while Ni particles could not be grafted onto SBA-15 in the absence of NH4OH (NH3/Ni mole ratio of 0). NH3/Ni mole ratio of 2~4 was suitable grafting conditions, which could give a product with the closest Ni amount to raw. This product obtained was named Ni-grafted SBA-15 sample. XPS, UV-vis and H2-TPR analyses demonstrated that a chemical bond was formed between Ni and silicon (Si) via oxygen (O), and no bulk nickel oxides existed in Ni-grafted SBA-15 sample. The formation of -O-Ni-O-Si-O-was completed via the reaction between hydrolyzate Ni(OH)(NH3)x-1) + from (Ni(NH3)x) 2+ and ≡Si-OH (silanol sites) on SBA-15 surface. Ni-grafted SBA-15 catalyst suited CO2 methanation, resulting in higher CO2 conversion and methane selectivity than NiO dispersed SBA-15 catalyst obtained by conventional post synthesis method. The activation energy for CO2 methanation increased with decreasing initial Ni amount used. The rate equation for CO2 methanation could be expressed as: r = kCCO 2 0.64 CH 2 4.05 , C was concentration. Ni-grafted SBA-15 catalyst had high thermal stability for CO2 methanation.