Coral reef lagoons are areas of complex carbon cycling, however, regional (e.g. land use) and global (e.g. climate) factors, including land runoff and ocean acidification, are adversely affecting carbonate-building coral reef systems. Coupled with this, surplus nutrients entering coastal waters can prompt excess algae growth, which can stimulate further carbon dioxide (CO2) production in the water column, thus enhancing coral/sediment dissolution. However, new inputs of alkalinity into coastal systems can buffer against acidification. By combining the natural groundwater tracer radon (222Rn) with carbonate chemistry in two contrasting Cook Island lagoons (the fringing Muri Lagoon on Rarotonga and the comparatively larger Aitutaki near-atoll lagoon), we were able to identify multiple drivers of coral reef acidification and regulation. Despite the lagoons having similar rates of submarine groundwater discharge (3.1 to 3.3 cm d−1; although the rate in Aitutaki is a maximum rate based on an assumed 100 m seepage face), groundwater inputs of CO2 and alkalinity were primarily driven by different sources (discrete offshore seeps in Muri Lagoon and dredged channels in Aitutaki Lagoon). Streams delivered low alkalinity water to both lagoons, but high pCO2 waters to the Aitutaki Lagoon in contrast to Muri Lagoon. Aragonite saturation states (ΩAr) ranged between 2.2 and 5.2, with areas of low ΩAr corresponding to areas of high radon and excess algal growth in Muri Lagoon, and areas that receive low alkalinity surface water in Aitutaki. Time-series sampling indicated that tidal heights and the ability of seawater to overtop the fringing reef influenced groundwater dynamics, lagoon hydrodynamics and carbonate chemistry. Groundwater discharge and stream flows were a significant freshwater source of new geologic CO2 and alkalinity to each lagoon, while recirculated seawater is likely a significant source of biologic CO2 driven by microbial respiration in sediments. The study found that while groundwater inputs of alkalinity may reduce acidification, they do not fully counteract ongoing acidification and CO2 inputs. This study also highlighted the need for future studies to undertake detailed spatial measurements to accurately characterise tropical island carbon dynamics due to the heterogeneous nature of these environments.