Amine-silica hybrid materials have been investigated extensively in terms of their suitability for postcombustion CO2 capture. However, research on how the silica types affects the synthesis and performance of amine-silica hybrid materials is scarce. In this study, four types of commonly used and representative silica including precipitated silica, fumed silica, MCM-41, and silica gel are used to synthesize a series of comparable materials by grafting a silane onto them. We undertake a porosity analysis of plain silica and the amine-silica hybrid materials and determined the CO2 adsorption performance of amine-silica hybrid materials. The results suggest that precipitated silica is a superior and promising support material for amine-silica hybrid materials synthesis by grafting. The amine-silica hybrid material supporting with precipitated silica possesses relatively high amine content, exhibits good porosity, and obtains the highest CO2 adsorption capacity and amine efficiency compared to those of three other amine-silica hybrid materials.