Revitalization of degraded landscapes may provide sinks for rising atmospheric CO2, especially in reconstructed prairies where substantial belowground productivity is coupled with large soil organic carbon (SOC) deficits after many decades of cultivation. The restoration process also provides opportunities to study the often-elusive factors that regulate soil processes. Although the precise mechanisms that govern the rate of SOC accrual are unclear, factors such as soil moisture or vegetation type may influence the net accrual rate by affecting the balance between organic matter inputs and decomposition. A resampling approach was used to assess the control that soil moisture and plant community type each exert on SOC and total nitrogen (TN) accumulation in restored grasslands. Five plots that varied in drainage were sampled at least four times over two decades to assess SOC, TN, and C4- and C3-derived C. We found that higher long-term soil moisture, characterized by low soil magnetic susceptibility, promoted SOC and TN accrual, with twice the SOC and three times the TN gain in seasonally saturated prairies compared with mesic prairies. Vegetation also influenced SOC and TN recovery, as accrual was faster in the prairies compared with C3-only grassland, and C4-derived C accrual correlated strongly to total SOC accrual but C3-C did not. High SOC accumulation at the surface (0–10 cm) combined with losses at depth (10–20 cm) suggested these soils are recovering the highly stratified profiles typical of remnant prairies. Our results suggest that local hydrology and plant community are critical drivers of SOC and TN recovery in restored grasslands. Because these factors and the way they affect SOC are susceptible to modification by climate change, we contend that predictions of the C-sequestration performance of restored grasslands must account for projected climatic changes on both soil moisture and the seasonal productivity of C4 and C3 plants.