Nowadays, one of the most distinguished subjects is the incrementation of CO₂ concentration that causes climate change. Based on the density functional theory analysis, structure, electronic, optical, and thermodynamic properties of four organic di-chalcogenide compounds such as C₁₁H₁₂NO₃Se–SeC₁₁H₁₂NO₃, C₉H₁₀NO₂Te–TeC₉H₁₀NO₂, C₁₂H₁₂NTe–TeC₁₂H₁₂N, and C₁₂H₁₂NSe–SeC₁₂H₁₂N, as candidates for carbon dioxide absorption, are investigated scientifically. The effect of different temperatures and various substitutions on the catalytic activity of the di-chalcogenide compounds in the capture and release of CO₂ has been investigated. The absorption spectrum of the di-chalcogen compounds has been obtained via the Ultraviolet–Visible optical spectra analysis. By the quantum theory of atoms in molecules and natural bond orbital analysis, the interaction between chalcogenide compounds and CO₂ has been evaluated. The positive effect of di-selenides compounds for capturing and releasing CO₂ has been represented in our investigation. The catalytic cycle of CO₂ capture and release is independent of the thermal effect. In contrast, the various substitutions of di-chalcogenide compounds directly influence the catalytic cycle of CO₂ capture and release.