The continuous release of carbon dioxide into the atmosphere will definitely cause damage to the environment. Environmental protection and reducing global warming are becoming very essential. The concentration of carbon dioxide in the atmosphere is due to the continuous burning of fossil fuels to attain the energy requirements. A novel method of adsorbing the most important greenhouse gas, carbon dioxide, using some ternary complex materials capable of adsorbing the gases effectively was studied. A ternary complex system with Zn (II) metal ion chelated with ampicillin (A) as the primary ligand and imidazole derivatives him/hist/his (B) as the secondary ligands ZnAB(B=hist/his)/ZnAB2 (B=him) species in all these systems were isolated, and the analytical data confirm its formation. Non-electrolytic behavior and monomeric types of chelates have been assessed from their low conductance values. The vibrational spectral data were interpreted to find the mode of binding of ligands to metal. The powder XRD and SEM analysis of the complexes suggest a nanocrystalline nature. The AFM images of selected complexes suggest mesoporous morphology, which has a higher tendency of adsorbing carbon dioxide gas. The ternary complexes exhibited surface areas ranging from 3.15 to 18.42 m²/g, with pore volumes of 0.004–0.008 cm³/g and average pore diameters of 5.8–2.6 nm. An excellent carbon dioxide uptake (20–38 wt%) was achieved at high temperature and pressure (303 K and 40 bar, respectively) using the ternary complexes. The ZnAB (B=his) ternary complex material exhibited the highest carbon dioxide uptake (38 wt%) due to its higher surface area and pore volume compared with the other two ternary complexes.