Herein, the synthesis of a new type of catalyst, SBA−M (Schiff complex of different metal types grafted on SBA‐15) based on a quaternization reaction, is described. Various amounts of ionic liquid were grafted into the pore channels of SBA‐15 using the post‐grafting method, which allowed the ionic liquid to be grafted into the pore channels restrictively. Notably, over six cycles, SBA−Mn (0.2) has been shown to maintain its catalytic activity and stability. In addition, a reaction mechanism for the cycloaddition of CO2 with epoxides based on density‐functional theory is proposed. The cycloaddition reaction of CO2 and epoxides is an efficient way of carbon fixation. It is demonstrated that the metal coordinated with the oxygen atom of the epoxides and that a halogen attacked the carbon of epoxides. Moreover, theoretical calculations and synthesis strategy provide a new approach for CO2 conversion.