To investigate the bioconcentration and potential health risks of metal(loid)s in a particular agro-ecological area, 230 pairs of soil and corresponding crop grain samples were collected from typical corn and wheat plants. The geo-accumulation index (Igeo), bioconcentration factors (BCF), health risk assessment (the target hazard quotient), and Receptor Prediction Model (PCS-SMLR) analysis were adopted to study the spatial distribution, assess the health risks, and predict the relationship between metal(loid)s and soil properties. It was found that the mean concentrations of Cu, Zn, Pb, Hg, and Cd in the study area’s agricultural soils exceeded the background soil concentrations, especially for Cd (0.2 mg/kg), Meanwhile, the corresponding Cd concentration in wheat samples was higher than the food quality limit. The results of the Igeo showed that the samples with a value higher than 0 for Cd and Hg accounted for 47.83% and 33.48%, respectively. The results of BCF of Cu, Zn, Cd, and As were higher in wheat than in corn, except for Ni. The target hazard quotient (TTHQ) of health risk of wheat, corn, and soil were higher for children (2.48) than adults (1.78), showing a potential health risk for individuals who mostly consume wheat. In addition, the PCS-SMLR analysis of the BCF prediction model for Cu, Zn, As, and soil properties showed differences in terms of the influences from wheat and corn. These results provide valuable information that not only can help local residents improve the staple food structure, but also can get provide a reference metal(loid)s concentration level for agricultural soils in the study area and restore a sustainable agro-ecological environment.