Because the CO2-calcite interface is of major importance in various environments and the energy industry, an accurate description of the adsorption kinetics of CO2 is critical for understanding the adsorption mechanisms involved. In this study, a new electrochemical method was implemented to unravel the adsorption kinetics of CO2 on a reconstructed calcite surface. In addition, an atomic simulation was used to provide details of the adsorbed interface. The results showed that the reconstructed calcite surface had different electrical conductivity under various conditions, which was attributed to differences in band gap values. The CO2 adsorption process on the reconstructed calcite surface was characterized by a change in electrical conductivity. Consequently, the adsorption rate constant at different temperatures and the energy barrier to be overcome in the gas adsorption process were obtained, with values of 0.0272-0.0412 s(-1) and 5.51 kJ/mol, respectively. This experimental result was well verified by molecular dynamics simulation. This study proved that the electrical conductivity of the material surface can accurately and quickly reflect the gas adsorption process, and the simulation method provided more details of the adsorption behavior at the gas-solid interface.