Reforestation has large potential for mitigating climate change through carbon sequestration. Native mixed-species plantings have a higher potential to reverse biodiversity loss than do plantations of production species, but there are few data on their capacity to store carbon. A chronosequence (5-45 years) of 36 native mixed-species plantings, paired with adjacent pastures, was measured to investigate changes to stocks among C pools following reforestation of agricultural land in the medium rainfall zone (400-800 mm yr-1) of temperate Australia. These mixed-species plantings accumulated 3.09 ± 0.85 t C ha-1 yr-1 in aboveground biomass and 0.18 ± 0.05 t C ha-1 yr-1 in plant litter, reaching amounts comparable to those measured in remnant woodlands by 20 years and 36 years after reforestation respectively. Soil C was slower to increase, with increases seen only after 45 years, at which time stocks had not reached the amounts found in remnant woodlands. The amount of trees (tree density and basal area) was positively associated with the accumulation of carbon in aboveground biomass and litter. In contrast, changes to soil C were most strongly related to the productivity of the location (a forest productivity index and soil N content in the adjacent pasture). At 30 years, native mixed-species plantings had increased the stability of soil C stocks, with higher amounts of recalcitrant C and higher C : N ratios than their adjacent pastures. Reforestation with native mixed-species plantings did not significantly change the availability of macronutrients (N, K, Ca, Mg, P, and S) or micronutrients (Fe, B, Mn, Zn, and Cu), content of plant toxins (Al, Si), acidity, or salinity (Na, electrical conductivity) in the soil. In this medium rainfall area, native mixed-species plantings provided comparable rates of C sequestration to local production species, with the probable additional benefit of providing better quality habitat for native biota. These results demonstrate that reforestation using native mixed-species plantings is an effective alternative for carbon sequestration to standard monocultures of production species in medium rainfall areas of temperate continental climates, where they can effectively store C, convert C into stable pools and provide greater benefits for biodiversity.