Soil has been identified as a possible carbon (C) sink to mitigate increasing atmospheric CO2 concentration. However, several recent studies have suggested that the potential of soil to sequester C is limited and that soil may become saturated with C under increasing CO2 levels. To test this concept of soil C saturation, we studied a gley and organic soil at a grassland site near a natural CO2 spring. Total and aggregate-associated soil organic C (SOC) concentration showed a significant increase with atmospheric CO2 concentration. An asymptotic function showed a better fit of SOC and aggregation with CO2 level than a linear model. There was a shift in allocation of total C from smaller size fractions to the largest aggregate fraction with increasing CO2 concentration. Litter inputs appeared to be positively related to CO2 concentration. Based on modeled function parameters and the observed shift in the allocation of the soil C from small to large aggregate-size classes, we postulate that there is a hierarchy in C saturation across different SOC pools. We conclude that the asymptotic response of SOC concentration at higher CO2 levels indicates saturation of soil C pools, likely because of a limit to physical protection of SOC.