Soil and land-management interactions in Australian native-forest regrowth remain a major source of uncertainty in the context of the global carbon economy. We sampled soil total organic C (TOC) and soil total N (TN) stocks at 45 sites within the Brigalow ecological community of the Brigalow Belt bioregion, Queensland, Australia. The sites were matched as triplets representing three land uses, specifically: uncleared native brigalow forest (‘Remnant’); grassland pasture (‘Pasture’), derived by clearing native vegetation and maintained as pasture for a minimum of 10 years, and; regrowing native brigalow forest (‘Regrowth’, stand ages ranging from 10 to 58 years) that had developed spontaneously after past vegetation clearing for pasture establishment. Soil TOC fractions and natural abundance of soil C and N isotopes were examined to obtain insight into C and N dynamics. An updated above- and belowground carbon budget for the bioregions was generated. Average soil TOC stocks at 0–0.3-m depth ranged from 19 to 79 Mg ha–1 and soil TN stocks from 1.8 to 7.1 Mg ha–1 (2.5th and 97.5th percentiles, respectively). A trend in stocks was apparent with land use: Remnant > Regrowth ≅ Pasture sites. Soil δ13C ranged from –14 to –27‰, and soil δ15N ranged from 4‰ to 17‰, in general reflecting the difference between Pasture (C4-dominated) land use and N2-fixing (C3-dominated) Remnant and Regrowth. Mid-infrared spectroscopy predicted C fractions as a percentage of soil TOC stock, which ranged from 5% to 60% (particulate), 20–80% (humus) and 9–30% (resistant/inert). The geo-referenced soil and management information we collected is important for the calibration of C models, for the estimation of national C accounts, and to inform policy developments in relation to land-resource management undertaken within the Brigalow Belt bioregions of Australia.