Owing to its wide availability, nontoxicity, and low cost, CO2 working as a trigger to reversibly switch material properties, including polarity, ionic strength, hydrophilicity, viscosity, surface charge, and degree of polymerization or cross-linking, has attracted an increasing attention in recent years. However, a quantitative correlation between basicity of these materials and their CO2 switchability has been less documented though it is of great importance for fabricating switchable system. In this work, the "switch-on" and "switch-off" abilities of melamine and its amino-substituted derivatives by introducing and removing CO2 are studied, and then their quantitative relationship with basicity is established, so that performances of other organobases can be quantitatively predicted. These findings are beneficial for forecasting the CO2 stimuli-responsive behavior of other organobases and the design of CO2-switchable materials.