The rise of modern Portland cement has relegated lime to a secondary role in the construction industry, now mainly used for repairing and restoring historical buildings. This study proposes an innovative application of partially calcined limestone (PCL) as a carbonated material. The impact of varying MgO dosages on the carbonation mechanism of PCL is explored. It is found that a 5% MgO dosage significantly enhances the 1 d compressive strength postcarbonation by over 84.7%. The critical role of hydrated MgCO 3 , produced from MgO, in the formation and crystallinity of CaCO 3 is highlighted. However, it is observed that excessive MgO can impede carbonation, negatively impacting the mechanical properties and pore structure of the material. The presence of MgCO 3 •3H 2 O is noted to significantly influence the compressive strength of the carbonated material. Potential pathways for dolomite formation in PCL with different MgO dosages are suggested, indicating new possibilities for creating high-performance, low-carbon cementitious materials.