Soils play an essential role in the global cycling of carbon and understanding the stabilisation mechanisms behind the preservation of soil organic carbon (SOC) pools is of globally recognised significance. Until recently, research into SOC stabilisation has predominantly focused on acidic soil environments and the interactions between SOC and aluminium (Al) or iron (Fe). The interactions between SOC and calcium (Ca) have typically received less attention, with fewer studies conducted in alkaline soils. Although it has widely been established that exchangeable Ca (CaExch) positively correlates with SOC concentration and its resistance to oxidation, the exact mechanisms behind this relationship remain largely unidentified. This synthesis paper critically assesses available evidence on the potential role of Ca in the stabilisation of SOC and identifies research topics that warrant further investigation. Contrary to the common view of the chemistry of base cations in soils, chemical modelling indicates that Ca2+ can readily exchange its hydration shell and create inner sphere complexes with organic functional groups. This review therefore argues that both inner- and outer-sphere bridging by Ca2+ can play an active role in the stabilisation of SOC. Calcium carbonate (CaCO3) can influence occluded SOC stability through its role in the stabilisation of aggregates; however, it could also play an unaccounted role in the direct sorption and inclusion of SOC. Finally, this review highlights the importance of pH as a potential predictor of SOC stabilisation mechanisms mediated by Al- or Fe- to Ca, and their respective effects on SOC dynamics.