Mining activities have increased the accumulation of heavy metals in farmland soil and in food crops. To identify the key soil properties influencing heavy metal bioavailability and accumulation in food crops, 81 crop samples and 81 corresponding agricultural soil samples were collected from rape, wheat, and paddy fields. Heavy metal (copper (Cu), zinc (Zn), lead (Pb), cadmium (Cd), iron (Fe), and manganese (Mn)) concentrations in soils and rape, wheat, rice grains were determined using inductively coupled plasma atomic emission spectroscopy, and soil physicochemical properties (pH, organic matter, total nitrogen, total phosphorus, available phosphorus, and available potassium (AK)) were analyzed. Soil extractable metals were extracted using various single extractants (DTPA, EDTA, NH4OAc, NH4NO3, and HCl). The average concentrations of Cu, Zn, Pb, Cd, and Mn in the soil samples all exceeded the local geochemical background value (background values of Cu, Zn, Pb, Cd, and Mn are 43.0, 81.0, 28.5, 0.196, and 616 mg/kg, respectively), and Cd over-standard rate was the highest, at 98%. Furthermore, soil total Cd concentrations (0.1–24.8 mg/kg) of more than 86% of the samples exceeded the soil pollution risk screening value (GB 15618-2018). The sources of Cu, Zn, Pb, Cd, and Mn in soils were mainly associated with mining activities. The key factors influencing heavy metal bioavailability were associated with the types of extractants (complexing agents or neutral salt extractants) and the metals. Cd and Pb concentrations in most wheat and rice grain samples exceeded the maximum allowable Cd and Pb levels in food, respectively, and Cd concentrations in approximately 10% of the rice grain samples exceeded 1.0 mg/kg. Furthermore, rice and wheat grains exhibited higher Cd accumulation capacity than rape grains, and despite the high soil Cd concentrations in the rape fields, the rape grains were safe for consumption. High soil pH and AK restricted Cd and Cu accumulation in wheat grains, respectively. Soil properties seemed to influence heavy metal accumulation in rice grains the most.
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