The relationship between the main physicochemical properties of soils and the accumulation of natural Zn and 65Zn radionuclide has been studied, and the capacity of soils to limit the mobility of the element in the soil–plant system has been assessed. The contribution of each of the selected soil state parameters to the accumulation of zinc by barley has been determined, and the soil state parameters have been ranked. It has been found that the largest contributions to the variation of the resulting parameter (65Zn accumulation coefficient, Ka) are made by mobile Fe (25%), free carbonates (21%), and acid-soluble Zn (18%). The largest contributions to the ZnacKa are made by free carbonates (13%) and mobile Fe (8%). The contributions of physical clay and organic carbon in soils and qualitative composition of humic substances are almost similar (4% for each). No differences in the inactivating capacity of different soils (soddy-podzolic soils, gray forest soils, and chernozems) for 65Zn are observed. This is related to the fact that the transfer of 65Zn to plants is statistically significantly controlled by the contents of free carbonates, mobile iron, and potentially plantavailable forms of stable natural Zn (carrier of 65Zn) rather than the quantitative and qualitative composition of organic matter and the degree of dispersion of mineral particles. The analysis of the ZnacKa/65Zn Ka ratios has shown that the share of plant-available Zn in the acid-soluble form of the metal (1 M HCl) is 0.61 on the average for the studied soils, and its share in the total Zn content in the soils is only 0.14.