In the United States (U.S.), the maintenance of forest cover is a legal mandate for federally managed forest lands. Reforestation is one option for maintaining forest cover on managed or disturbed lands, and as a land use change can increase forest cover on previously non-forested lands, enhancing carbon (C)-based ecosystem services and functions such as the production of woody biomass for forest products and the mitigation of atmospheric CO₂ pollution and climate change. Nonetheless, multiple assessments indicate that reforestation in the U.S. lags behind its potential, with continued 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. Here, we report the findings of a large-scale data synthesis aimed at four objectives: 1) estimate C storage in major pools in forest and other land cover types; 2) quantify sources of variation in C pools; 3) compare the impacts of reforestation and afforestation on C pools; 4) assess whether results hold or diverge across ecoregions. Our data-driven analysis provides four key inferences regarding reforestation and other land use impacts on C sequestration. First, soils are the dominant C pool under all land cover types in the U.S., and spatial variation in soil C pool sizes has less to do with land cover than with other factors. Second, where historically cultivated lands are being reforested, topsoils are sequestering significant amounts of C, with the majority of reforested lands yet to reach sequestration capacity (relative to forested baseline). Third, the establishment of woody vegetation delivers immediate to multi-decadal C sequestration benefits in biomass and coarse woody debris pools, with two- to three-fold C sequestration benefits during the first several decades following planting. Fourth, opportunities to enhance C sequestration through reforestation vary among 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.