Changes in carbon stocks and physical properties of gray forest soils during their postagrogenic evolution have been studied in the succession chronosequence comprising an arable, lands abandoned 6, 15, and 30 years ago; and a secondary deciduous forest (Experimental Field Station of the Institute of Physicochemical and Biological Problems of Soil Science, Russian Academy of Sciences, Pushchino, Moscow region). It is found that carbon stocks in the upper 60-cm soil layer gain with increasing period of abandonment, from 6.17 kg C/m2 on the arable land to 8.81 kg C/m2 in the forest soil, which represents the final stage of postagrogenic succession. The most intensive carbon accumulation occurs in the upper layer of the former plow (0- to 10-cm) horizon. It is shown that the self-restoration of gray forest soils is accompanied by a reliable decrease of bulk density in the upper 10-cm layer from 1.31 ± 0.01 g/cm3 on the arable to 0.97 ± 0.02 g/cm3 in the forest. In the former plow horizon of the arable–abandoned land–forest succession series, the portion of macroaggregates increases from 73.6 to 88.5%; the mean weighted diameter of aggregates, by 1.6 times; and the coefficient of aggregation, by 3.8 times. Thus, the removal of lands from agricultural use results in a gradual restoration of their natural structure, improvement of soil agronomical properties, and carbon sequestration in the upper part of the soil profile. © 2017, Pleiades Publishing, Ltd.