A sound understanding of the sustainability of terrestrial carbon (C) sequestration is critical for the success of any policies geared toward stabilizing atmospheric greenhouse concentrations. This includes the Kyoto Protocol and/or other greenhouse strategies implemented by individual countries. However, the sustainability of C sinks and pools has not been carefully studied with either empirical or theoretical approaches. This study was intended to develop a conceptual framework to define the sustainability based on C influx and residence time (τ). The latter τ quantifies the capacity for C storage in various plant and soil pools. We estimated τ via inverse analysis of multiple data sets from a Free-Air CO2 Enrichment (FACE) experiment in Duke Forest, North Carolina, United States. This study suggested that estimated residence times at elevated CO2 decreased for plant C pools and increased for litter and soil pools in comparison to those at ambient CO2. The ensemble of the residence times from all the pools at elevated CO2, however, was well correlated with that at ambient CO2. We then used the estimated residence times, combined with C influx, to simulate C sequestration rates in response to a gradual increase in atmospheric CO2 concentration (Ca). The simulated C sequestration rate gradually increased from 69 g m-2 yr-1 in 2000 when Ca was 378 ppm to 201 g m-2 yr-1 in 2100 when Ca was at 710 ppm. Thus, the current evidence from both experimental observations and inverse analysis suggested that C sequestration in the forest ecosystem was likely to increase gradually as Ca gradually increases. The model projection of the C sequestration will improve as more data on long-term processes become available in coming years. In addition, such a modeled increase in terrestrial C sequestration is too small to balance the anthropogenic C emission.