Calcite is one of the most abundant components of the Earth’s crust, constituting the largest carbon reservoir in the global carbon cycle. Thus, large-scale dissolution of calcite would have enormous impact on the weather, geography and aquatic environment, for example, changes in the carbon dioxide concentration of the air and the acidity of the ocean. The dissolution mechanism of calcite has importance in geologic carbon sequestration (GCS) technology to capture carbon dioxide from the air and to store it underground. In order to precisely predict such a large-scale and long-term phenomenon, the dissolution mechanism of calcite should be understood at an atomic level in a precise manner.