Soil organic carbon (SOC) sequestration is important for improving soil fertility of cropland and for the mitigation of greenhouse gas emissions to the atmosphere. The efficiency of SOC sequestration depends on the quantity and quality of the organic matter, soil type, and climate. Little is known about the SOC sequestration efficiency of organic amendments in Vertisols. Thus, we conducted the research based on 29 years (1982–2011) of long-term fertilization experiment with a no fertilizer control and five fertilization regimes: CK (control, no fertilizer), NPK (mineral NPK fertilizers alone), NPK+1/2W (mineral NPK fertilizers combined with half the amount of wheat straw), NPK+W (mineral NPK fertilizers combined with full the amount of wheat straw), NPK+PM (mineral NPK fertilizers combined with pig manure) and NPK+CM (mineral NPK fertilizers combined cattle manure). Total mean annual C inputs were 0.45, 1.55, 2.66, 3.71, 4.68 and 6.56 ton/ha/yr for CK, NPK, NPKW1/2, NPKW, NPKPM and NPKCM, respectively. Mean SOC sequestration rate was 0.20 ton/ha/yr in the NPK treatment, and 0.39, 0.50, 0.51 and 0.97 ton/ha/yr in the NPKW1/2, NPKW, NPKPM, and NPKCM treatments, respectively. A linear relationship was observed between annual C input and SOC sequestration rate (SOCsequestration rate = 0.16 Cinput –0.10, R = 0.95, P<0.01), suggesting a C sequestration efficiency of 16%. The Vertisol required an annual C input of 0.63 ton/ha/yr to maintain the initial SOC level. Moreover, the C sequestration efficiencies of wheat straw, pig manure and cattle manure were 17%, 11% and 17%, respectively. The results indicate that the Vertisol has a large potential to sequester SOC with a high efficiency, and applying cattle manure or wheat straw is a recommendable SOC sequestration practice in Vertisols.