The paired Fluvisol and cereal samples in both the field screening and controlled experiments are reported to elucidate the soil–crop relationship for As, Cd, and Pb in relation to changing contamination levels. Significant varietal differences in plant uptake were observed for crop type (barley, triticale) and the harvested part of the crop (oat shoots and grain). When parametrizing the stepwise regression models, the inclusion of soil properties often improved the performance of soil–crop models but diverse critical soil parameters were retained in the model for individual metal(loid)s. The pH value was often a statistically significant variable for Cd uptake. For As and Pb, the more successful model fit was achieved using the indicators of quantity or quality of soil organic matter, but always with lower inherent model reliability compared to Cd. Further, a single correlation analysis was used to investigate the relationship between extractable metal concentrations in soil solution and their crop accumulation. For Cd, there were strong intercorrelations among single extractions, the NH4NO3 extraction stood out with perfect correlation with plant uptake in both experiments. For As and Pb, the CaCl2 and Na2EDTA solutions outperformed other single extractions and were the better choice for the assessment of depositional fluvial substrates.
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