The recent industrial revolution and increasing human population demands sufficient amount energy resource for which we ultimately depend on fossil fuels. Usage of fossil fuel results in emission of CO2 gas which causes global warming. Indeed, in early earth history, natural sequestration of dissolved CO2 can be observed by the formation of secondary calcium carbonate (calcite) and secondary magnesium carbonate (magnesite). However, due to the increasing CO2 concentration in atmosphere, alternate CO2 capture and storage technologies have been explored to arrest CO2 during the post-, pre- and oxy-combustion processes itself. Hence, current interests of scientist focus to capture and control technology. Particularly, CO2 capture and separation technologies comprise of amine solvents, PEI membranes, ionic liquids, MOFs, metal oxides etc. Recently, an enzyme-based system, which achieves CO2 capture and release by mimicking the mechanism of the mammalian respiratory system, is under development. Accordingly, this study deals immobilization of enzyme carbonic anhydrase (CA) on functionalized and metal nanoparticles confined mesoporous silica for CO2 hydration and its sequestration to CaCO3. From various experimental studies, it is concluded that the immobilized CA retains about 90% of enzymatic activity more than 20 cycles. It is also concluded that the storage stability and thermal stability of immobilized CA is better than those of free enzymes. The immobilized CAs are green materials, and are tunable, reusable, and promising biocatalysts for CO2 sequestration.