A dual-templated MgO-Al2O3 (denoted as SI-MA) was prepared by a single-step evaporation-induced self-assembly (EISA) method using P123 and ionic liquid as template. For comparison, P123-templated MgO-Al2O3 (denoted as S-MA) and ionic liquid-templated MgO-Al2O3 (denoted as I-MA) were also prepared by a similar method. The effect of P123 and ionic liquid on physicochemical properties and CO2 adsorptive performance of adsorbents was investigated. All the adsorbents retained well developed mesoporous structure and SI-MA exhibited the highest surface area. It was observed that relative distribution of coordinately unsaturated aluminum increased in the order of I-MA < SI-MA < S-MA. Similarly, the basicity of adsorbent increased in the order of I-MA < S-MA < SI-MA and the highest basicity of SI-MA was due to its highest surface area and the large amount of coordinately unsaturated O2- ions. It was also revealed that the CO2 adsorption capacity under dynamic conditions, decreased in the order of SI-MA > S-MA > I-MA, which is in accordance with the trend of basicity. In conclusion, it was found that SI-MA with the highest basicity retained the maximum CO2 adsorptive performance demonstrating that the basicity of the adsorbents played an important role in determining CO2 adsorption capacity. (C) 2015 Elsevier B.V. All rights reserved.