The potential for mitigating increasing atmospheric carbon dioxide concentrations through the use of terrestrial biological carbon (C) sequestration is substantial. Here, we estimate the amount of C being sequestered by natural processes at global, North American, and national US scales. We present and quantify, where possible, the potential for deliberate human actions - through forestry, agriculture, and use of biomass-based fuels - to augment these natural sinks. Carbon sequestration may potentially be achieved through some of these activities but at the expense of substantial changes in land-use management. Some practices (eg reduced tillage, improved silviculture, woody bioenergy crops) are already being implemented because of their economic benefits and associated ecosystem services. Given their cumulative greenhouse-gas impacts, other strategies (eg the use of biochar and cellulosic bioenergy crops) require further evaluation to determine whether widespread implementation is warranted. Front Ecol Environ 2012; 10(10): 554-561, doi:10.1890/120065