Soil organic matter pools under contrasting long-term management systems provide insight into potentials for sequestering soil C, sustaining soil fertility and functioning of the soil–atmospheric interface. We compared soil C and N pools (total, particulate and microbial) under pastures (1) varying due to harvest technique (grazing or haying), species composition (cool- or warm-season), stand age and previous land use and (2) in comparison with other land uses. Grazed tall fescue-common bermudagrass pasture (20 yr old) had greater soil organic C (31%), total N (34%), particulate organic C (66%), particulate organic N (2.4 fold) and soil microbial biomass C (28%) at a depth of 0–200 mm than adjacent land in conservation-tillage cropland (24 yr old). Soil organic C and total N at a depth of 0–200 mm averaged 3800 and 294 g m−2, respectively, under grazed bermudagrass and 3112 and 219 g m−2, respectively, under hayed bermudagrass. A chronosequence of grazed tall fescue suggested soil organic N sequestration rates of 7.3, 4.4 and 0.6 g m−2 yr−1 to a depth of 200 mm during 0–10, 10–30 and 30–50 yr, respectively. Soil C storage under long-term grazed tall fescue was 85 to 88% of that under forest, whereas soil N storage was 77 to 90% greater under grazed tall fescue than under forest. Properly grazed pastures in the Southern Piedmont USA have great potential to restore natural soil fertility, sequester soil organic C and N and increase soil biological activity.