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Inorganic pollution induced by smelting waste has threatened the safety of environment, whereas the impacts on farmlands with regards to potentially toxic elements (PTEs) receive insufficient attention. Herein, the contents, transfer pathways and potential risks of the PTEs in common crops were examined from different farmlands distributed around an indigenous Zn-smelting area in Guizhou, China. The results showed that Tl in cabbage (Brassica oleracea L.) (up to 3.74 mg/kg) and radish (Raphanus sativus L.) (up to 1.16 mg/kg) at some sites exceeded the maximum permissible level (MPL) (0.5 mg/kg) for food, and, under the same pollution condition, cabbage and radish were more likely to enrich PTEs, and the edible portion of maize was not prone to Tl risk. Hazard quotient calculations of Tl, Ba, and U were greater than 1, indicating the edible risk of crops for these PTEs. Further characterization of selected soils revealed that MnFe 2 O 4 and Fe 2 O 3 controlled the phase transformation of Tl(III) in rhizospheric soils. Furthermore, distinctive mullite was detected in the soil which confirmed the contribution of high temperature smelting to PTEs pollution. The findings indicate an emergent need for soil remediation around historical indigenous metal smelting areas for the sake of food security. [Display omitted] • Visibly elevated thallium (Tl) contents were observed in some crops at site CS-5. • Iron oxides may affect the phase transformation of Tl(I)–Tl(III) in rhizospheric soils. • Some species of the studied crops may exert a non-negligible health risk for consumers. [ABSTRACT FROM AUTHOR]