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The elevated accumulation of cadmium (Cd) in rice (Oryza sativa L.) and tea (Camellia sinensis L.) grown in agricultural soils may lead to a variety of adverse health effects. This study collected and analyzed crop samples along with paired rhizosphere soil samples from 61 sites in Cd-contaminated regions in Anhui Province, China. The findings revealed that both the diffusive gradients in thin-films (DGT) and soil solution were capable of effectively predicting Cd contents in crops. Conventional chemical extraction methods were inappropriate to evaluate the bioavailability of Cd. However, the effective concentrations (CE) corrected by the DGT-induced fluxes in soils (DIFS) model exhibited the strongest correlation with crop Cd contents. Except for CE, various measurement methods yielded better results for predicting Cd bioavailability in tea compared to rice. Pearson's correlation analysis and the random forest (RF) model identified the key influencing factors controlling Cd uptake by rice and tea, including pH, soil texture, and contents of zinc (Zn) and selenium (Se) in soils, which antagonize Cd. To reduce the potential health risk from rice and tea, the application of soil liming and/or Se-oxidizing bacteria was expected to be an effective management strategy. [ABSTRACT FROM AUTHOR]