Amine-grafted MSU-3 mesoporous silica samples were synthesized from pure and waste silica sources and their CO2 adsorption performances were evaluated. The obtained samples were characterized using X-ray diffraction (XRD), thermogravimetric analysis (TGA), N2 adsorption–desorption isotherm analysis, Fourier transform infrared (FTIR), and transmission electron microscopy (TEM). CO2 adsorption capacities of the samples at different temperatures were determined by TGA. The amine-modified MSU-3 synthesized from waste exhibited the highest CO2 adsorption capacity of 1.32 mmol/g at 25 °C and 1 bar, depending essentially on the porous texture and the amine content of the material. The CO2 adsorption isotherms of the synthesized samples were measured by a static volumetric method. Adsorption isotherm indicated that the amine-modified samples presented significantly higher CO2 adsorption capacity than the pure samples. The Avrami kinetic model fitted the experimental data well and suggested that complex reaction mechanism or the appearance of multiple reaction pathway occurred in the CO2 adsorption.