A series of CO2 adsorbents were synthesized by functionalizing SBA-15 via stepwise growth of amine-terminated melamine-based dendrimers. The adsorbents contained very high organic loadings (up to 50.3 wt % ) relative to previous reports. In addition to that, CO2 adsorption measurements demonstrated that primary amine groups are the only active groups within these dendritic structures for CO2 adsorption. The CO2 adsorption capacities of these adsorbents (except for fourth generation dendrimer functionalized SBA-15) are improved relative to the unfunctionalized SBA-15. The exception is associated with the completely filled pores of this adsorbent.