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Tetraethylenepentamine (TEPA) was employed to functionalize the large-pore mesoporous silica (denoted MSU-J) with 3D worm-hole framework structures which was prepared through a supramolecular hydrogen-bonding assembly pathway from low-cost H 2 NCH(CH 3 )CH 2 [OCH 2 CH(CH 3 )] 33 NH 2 (D2000) as structure-directing porogens and tetraethylorthosilioate as the silica source for capturing CO 2 . The resultant adsorbents were characterized by FT-IR, Transmission electron microscopy (TEM), N 2 adsorption/desorption and thermogravimetric analysis. Textural properties, elemental analysis and TEM measurement of the samples showed a severe pore filling of MSU-J as TEPA loading was increased to 70 wt%. CO 2 adsorption isotherms measured at different temperatures revealed the optimal adsorption temperature is 25°C. The adsorption capacity of MSU-J with different TEPA loading contents was calculated. As a result, 50 wt% of TEPA supported on as-synthesized MSU-J achieved the highest capacity with the value of 164.3 mg/g under the conditions of 99.99 % CO 2 at 25°C and 0.1 MPa. Repeated adsorption/desorption cycles revealed that amine-impregnated materials was very efficient for less apparent decrease in CO 2 adsorption capacity even after 6 adsorption-regeneration cycles.