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Arable land soils generally have lower organic carbon (C) levels than soils under native vegetation; increasing the C stocks through improved management is suggested as an effective means to sequester CO2 from the atmosphere. China's arable lands, accounting for 13% of the world's total, play an important role in soil C sequestration, but their potential to enhance C sequestration has not yet been quantitatively assessed. The C sequestration by agricultural soils is affected by many environmental factors (such as climate and soil conditions), biological processes (crop C fixation, decomposition and transformation), and crop and soil management (e.g. tillage and manure application). Estimation of the C sequestration potential requires the quantification of the combined effects of these factors and processes. In this study, we used a coupled remote sensing- and process-based ecosystem model to estimate the potential for C sequestration in agricultural soils of China and evaluated the sustainability of soil C uptake under different soil management options. The results show that practicing no-tillage on 50% of the arable lands and returning 50% of the crop residue to soils would lead to an annual soil C sequestration of 32.5 Tg C, which accounts for about 4% of China's current annual C emission. Soil C sequestration with improved soil management is highly time-dependent; the effect lasted for only 20-80 years. Generally, practicing no-tillage causes higher rate and longer sustainability of soil C sequestration than only increasing crop residue into soils. The potential for soil C sequestration varied greatly among different regions due to the differences in climate, soil conditions and crop productivity.