Trimodal nanoporous silica (TS) was studied as a support for solid amine CO2 sorbent. The advantages of TS over mesoporous silica as the amine support was evaluated. Amine-functionalized TS showed advantages in CO2 adsorption capacity and kinetics. Amine-functionalized as-prepared TS showed promising for CO2 capture. The advantages of TS as the amine support was due to its textural properties.