Adsorption technology is a well-established technology for CO2 removal. MSU-2 mesoporous silica appears to be very potential adsorbent for efficient CO2 gas adsorption due to its three-dimensional (3D) wormhole framework structures that are highly interconnected which is able to minimize the diffusion resistance of CO2. So far, there is no previous study reported on the CO2 adsorption of MSU-2. Thus, the current study focuses on the investigation on the synthesis of MSU-2 by using different surfactants (Triton X-100, Igepal CA-720 or Tergitol NP-9) and followed by the CO2 adsorption studies on the synthesized MSU-2. The morphology, crystallinity, functional groups, pore characteristics and pore structure of the MSU-2 synthesized were investigated. FESEM images showed that MSU-2 synthesized by using Igepal CA-720 possessed the most uniform and defined microspherical morphology compared to the MSU-2 synthesized by using the other surfactants. Besides, the MSU-2 synthesized by using Igepal CA-720 displayed the highest BET surface area of 938 m2/g and CO2 adsorption capacity of 0.57 mmol/g compared to the other MSU-2 samples. The obtained results showed that Igepal CA-720 is the most suitable surfactant for MSU-2 synthesis compared to the other surfactants in the current study. © 2019 Taylor & Francis Group, LLC.