Without Al modified SBA-15 as template, the CMK-5 (ordered mesoporous carbon) material was easily synthesized. The SBA-15 (ordered mesoporous silica) material and oxalic acid were respectively used as template and the polymerization catalyst. The ordered bimodal mesoporous structure of the synthesized CMK-5 sample was tested by nitrogen adsorption/desorption data at 77 K, TEM, SEM, XRD and Raman analysis. The SBET surface area, V (pore volume) and bimodal diameters of the synthesized CMK-5-0.75 material were respectively 1475 m2/g, 1.93 cm3/g, 4.2 nm and 2.8 nm. The CO2 capture performance of the CMK-5-0.75 material was tested. The CO2 capture capacities of the dry CMK-5-0.75 material and the wet CMK-5-0.75 material (Rw = 3.5) individually reached 30.0 mmol/g and 57 mmol/g at 3.2 MPa and 275 K. The CO2 capture behaviors of several ordered mesoporous samples were compared, and the CMK-5-0.75 material was the best CO2 capture material among them.