Field experiments on the decomposition of organic materials and the accumulation of organic carbon in infertile red soils were conducted at the Ecological Experimental Station of Red Soil, the Chinese Academy of Sciences, and the potential of CO2 sequestration by reclamation and improving the fertility of these soils was estimated. Results showed that in infertile red soils, the humification coefficients of organic materials were rather high, ranging from 0.28 to 0.63 with an average of 0.43, which was 41% higher than those in corresponding red soils with medium fertility. This was mainly attributed to the high clay content, high acidity and low native organic matter content of infertile red soils. Compared to those in corresponding normal red soils, the decomposition rates of organic materials were significantly lower in infertile red soils in the first 2 years, thereafter no significant difference was observed between those in the two kinds of soils.Depending on the kind and amount of organic manure applied, the soil properties and the rotation systems,annual application of organic manure with a rate of 4 500 to 9 000 kg ha-1 increased the organic carbon content in surface 20 cm of infertile red soils by 2.1～7.5 g kg-1 with an average of 4.7 g kg-1 within the first 5 years. The organic carbon content in infertile red soils which received organic manure annually increased linearly in the first 10 years, thereafter it slowed down, implying that the fertility of the infertile red soils could reach middle or high level in 10 years if the soil was managed properly. It was estimated that through exploitation of wastelands, re-establishment of fuel forests and improvement of soil fertility, soils in red soil region of China could sequester an extra 1.50×1015 g of atmospheric CO2.