Soil organic carbon (SOC) is the largest terrestrial carbon (C) sink on Earth; this pool plays a critical role in ecosystem processes and climate change. Given the cost and time required to measure SOC, and particularly changes in SOC, many signatory nations to the United Nations Framework Convention on Climate Change report estimates of SOC stocks and stock changes using default values from the Intergovernmental Panel on Climate Change or country-specific models. In the United States, SOC in forests is monitored by the national forest inventory (NFI) conducted by the Forest Inventory and Analysis (FIA) program within the U.S. Department of Agriculture, Forest Service. The FIA program has been consistently measuring soil attributes as part of the NFI since 2001 and has amassed an extensive inventory of SOC in forest land in the conterminous United States and southeast and southcentral coastal Alaska. That said, the FIA program has been using country-specific predictions of SOC based, in part, upon a model using SOC estimates from the State Soil Geographic (STATSGO) database compiled by the Natural Resources Conservation Service. Estimates obtained from the STATSGO database are averages over large map units and are not expected to provide accurate estimates for specific locations, e.g., NFI plots. To improve the accuracy of SOC estimates in U.S. forests, NFI SOC observations were used for the first time to predict SOC density to a depth of 100 cm for all forested NFI plots. Incorporating soil-forming factors along with observations of SOC into a new estimation framework resulted in a 75% (48 ± 0.78 Mg/ha) increase in SOC densities nationally. This substantially increases the contribution of the SOC pool, from approximately 44% (17 Pg) of the total forest ecosystem C stocks to 56% (28 Pg), in the forest C budget of the United States.