In the United States (U.S.), the maintenance of forest cover is a legal mandate for federally managed forest lands. More broadly, reforestation following harvesting, recent or historic disturbances can enhance numerous carbon (C)-based ecosystem services and functions. These include production of woody biomass for forest products, and mitigation of atmospheric CO2 pollution and climate change by sequestering C into ecosystem pools where it can be stored for long timescales. Nonetheless, a range of assessments and analyses indicate that reforestation in the U.S. lags behind its potential, with the continuation of ecosystem services and functions at risk if reforestation is not increased. In this context, there is need for multiple independent analyses that quantify the role of reforestation in C sequestration, from ecosystems up to regional and national levels. Here, we describe the methods and report the findings of a large-scale data synthesis aimed at four objectives: (1) estimate C storage in major ecosystem pools in forest and other land cover types; (2) quantify sources of variation in ecosystem C pools; (3) compare the impacts of reforestation and afforestation on C pools; (4) assess whether these results hold or diverge across ecoregions. The results of our synthesis support four overarching inferences regarding reforestation and other land use impacts on C sequestration. First, in the bigger picture, soils are the dominant C pool in all ecosystems and land cover types in the U.S., and soil C pool sizes vary less by land cover than by other factors, such as spatial variation or soil wetness. Second, where historically cultivated lands are being reforested, topsoils are sequestering significant amounts of C, with the majority of reforested lands yet to reach their capacity relative to the potential indicated by natural forest soils. Third, the establishment of woody vegetation delivers immediate to multi-decadal C sequestration benefits in aboveground woody biomass and coarse woody debris pools, with two- to three-fold C sequestration benefits in biomass during the first several decades following planting. Fourth, opportunities to enhance C sequestration through reforestation vary among the ecoregions, according to current levels of planting, typical forest growth rates, and past land uses (especially cultivation). Altogether, our results suggest that an immediate, but phased and spatially targeted approach to reforestation can enhance C sequestration in forest biomass and soils in the U.S. for decades to centuries to come.