In addition to non-hydraulic lime, natural hydraulic lime (NHL) is a material widely used to repair and restore historic buildings. In Korea, although lime mortars have been used as important building materials for thousands of years, the sharing of information and technology with other countries has been relatively inactive. While not recognizing the suitability of NHL as a repair material, undesirable materials such as Portland cement have often been selected due to their high strength, ease of use, and hydraulicity, but unfortunately, this has resulted in the irreversible damage of existing elements, especially in historic masonry structures. This study aims to emphasize the need for hydraulic lime for the sustainable preservation of Korea’s architectural heritage. To justify its use, historical and scientific investigations were conducted. By reviewing literature written in the 15th century, it was found that dark limestone was used to manufacture building lime. Based on this, the chemical compositions of different-colored limestone were experimentally analyzed, and significant evidence was found that dicalcium silicate was formed in the quicklime manufactured by calcining blue-green and green-black limestone. Prior to the 19th century, it would have been impossible to record the chemical compositions of various types of limestone, except for visual observations such as color differences. Fortunately, this important information was recorded in royal documents and has been handed down to the present day. Thus, knowledge from 500 years ago could be scientifically interpreted using the latest technology. The link between the historical record and the experimental results shown in this study can contribute to the selection of a suitable material. This is a method for the preventive preservation of historic masonry structures, as it can significantly lower the possibility of future damages caused by efflorescence and freeze–thaw.