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Cenospheres (CS) are spherical shaped inorganic frameworks present in with fly ash which is generated from coal-fired thermal power plants. These spherical structures were functionalized with imidazole and amine moieties to capture CO 2 selectively from flue gases at elevated temperature. The functionalized CS have shown a high selectivity for CO 2 adsorption (4.68 mmol g -1 ) over N 2 (0.46 mmol g -1 ) at 333 K/1 bar from a simulated flue gas (0.15 CO 2 and 0.85 N 2 , v%) composition of thermal power plants. When the moisture content reached to 30 vol% the adsorption capacity of CS materials was reduced to 20 vol% as compared to dry flue gas. The functionalized CS can be used repeatedly for 50 cycles without losing its adsorption capacity. The cost estimate for CO 2 capture by using the proposed adsorption system would be $12.01/ton of CO 2 which is lower as compared to amine absorption system and zeolite-based adsorption system reported in the literature. The CS materials are prepared from solid wastes reduce the cost of production and their large scale manufacturing is technically feasible to capture CO 2 from industrial flue gases efficiently in near future., (Copyright © 2021 Elsevier Ltd. All rights reserved.)