CO2 capture from industrial processes and power plants, contribute to curbing global warming and advancing sustainability efforts. This study involves the design and synthesis of novel mesoporous silica supported ionic liquid based adsorbents for carbon dioxide capture. Utilization of MSILs delves into the efficiency and mechanisms of CO2 adsorption, offering insights for sustainable carbon capture technologies in combating greenhouse gas emissions. 1-ethyl-3-methylimidazolium tetrafluoroborate, 1-ethyl-3-methylimidazolium ethyl sulfate and 1-ethyl-3-methylimidazolium methylsulfate ionic liquids were anchored on the surface of mesoporous silica which then led to highly efficient adsorbent material. Simple, efficient and cost saving methodology was performed to synthesize such highly efficient CO2 adsorbent materials. In addition, we theoretically predicted the favorable interaction mechanism of chosen molecular entities for CO2 adsorption using density functional theory (DFT) analysis. Theoretical results depict the strong interaction of molecular entities with CO2 gas molecules which is clearly evident from the experimental findings.