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Hexavalent chromium [Cr(VI)]-contaminated soils have introduced a serious problem in China. Cr(VI) is hazardous to both the environment and public health and may degrade the engineering properties of soils. Accordingly, the effects of Cr(VI) on the physicochemical, mechanical, and microstructure properties of Chinese clay were investigated in this study. Results show that Cr(VI) had a considerable negative effect on the physicochemical, mechanical, and microstructure properties of soil. Specifically, Cr(VI) changed the physicochemical properties and degraded the mechanical properties of soil, led to the aggregation of soil particles, and created a large void space. Cr(VI) also changed the mineral composition of the soil and converted clay minerals into calcite. The changes in the microstructure and mineral composition of the soil were the primary reasons for the differences in the engineering properties of Cr(VI)-contaminated soil.