A quantitative understanding of the rate at which land ecosystems are sequestering or losing carbon at national-, regional-, and state-level scales is needed to develop policies to mitigate climate change. In this study, a new improved historical land use and land cover change data set is developed and combined with a process-based ecosystem model to estimate carbon sources and sinks in land ecosystems of the conterminous United States for the contemporary period of 2001–2005 and over the last three centuries. We estimate that land ecosystems in the conterminous United States sequestered 323?Tg?C?yr?1 at the beginning of the 21st century with forests accounting for 97% of this sink. This land carbon sink varied substantially across the conterminous United States, with the largest sinks occurring in the Southeast. Land sinks are large enough to completely compensate fossil fuel emissions in Maine and Mississippi, but nationally, carbon sinks compensate for only 20% of U.S. fossil fuel emissions. We find that regions that are currently large carbon sinks (e.g., Southeast) tend to have been large carbon sources over the longer historical period. Both the land use history and fate of harvested products can be important in determining a region's overall impact on the atmospheric carbon budget. While there are numerous options for reducing fossil fuels (e.g., increase efficiency and displacement by renewable resources), new land management opportunities for sequestering carbon need to be explored. Opportunities include reforestation and managing forest age structure. These opportunities will vary from state to state and over time across the United States.