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Simple Summary: After the collapse of the Soviet Union, changes in the agricultural structure led to widespread abandonment of cropland and natural vegetation restoration in Russia, Ukraine, and Belarus. In consequence, corresponding changes in the terrestrial carbon cycle need to be quantified. We simulated this process using a dynamic vegetation model, and found that the conversion of cropland to natural vegetation generally formed a significant carbon sink at 0.99 GtC; the growth of the vegetation carbon pool, especially, was significantly higher than that of soil carbon pool. Land use and cover changes (LUCC) have a fundamental impact on the terrestrial carbon cycle. The abandonment of cropland as a result of the collapse of the Soviet Union offers a typical case of the conversion from cropland to natural vegetation, which could have a significant effect on the terrestrial carbon cycle. Due to the inaccuracy of LUCC records, the corresponding impact on the terrestrial carbon cycle has not been well quantified. In this study, we estimated the carbon flux using the Vegetation-Global-Atmosphere-Soil (VEGAS) model over the region of Russia, Belarus and Ukraine during 1990–2017. We first optimized the LUCC input data by adjusting the Food and Agriculture Organization (FAO) data by Russian statistical data and redistributing the spatiotemporal input data from the Historical Database of the Global Environment (HYDE) to the original model. Between 1990 and 2017, the area of cropland abandonment was estimated to be 36.82 Mha, compared to 11.67 Mha estimated by FAO. At the same time, the carbon uptake from the atmosphere to the biosphere was 9.23 GtC (vs fixed cropland 8.24 and HYDE 8.25 GtC) during 1990–2017, which means by optimizing the cropland distribution data, the total carbon absorption during the abandonment process increased by 0.99 GtC. Meanwhile, the growth of the vegetation carbon pool was significantly higher than that of the soil carbon pool. Therefore, we further highlight the importance of accurate cropland distribution data in terrestrial carbon cycle simulation. [ABSTRACT FROM AUTHOR]