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It is a daunting challenge to predict toxicity and accumulation of rare earth metals (REMs) in different exposure scenarios (e.g., varying water chemistry and metal combinations). Herein, we investigated the toxicity and uptake of La and Ce in the presence of various levels of Ca, Mg, Na, K, and at different pH values, as well as the combined effects of La and Ce in wheat Triticum aestivum. Major cations (Ca2+ and Mg2+) significantly mitigated the toxicity and accumulation of La3+/Ce3+. Toxicity and uptake of La, Ce, and La-Ce mixtures could be well quantified by the multi-metal biotic ligand model (BLM) and by the Langmuir-type uptake model with the consideration of the competitive effects of Ca2+ and Mg2+, with more than 85.1% of variations explained. The derived binding constants of Ca, Mg, La, and Ce to wheat root were respectively 3.87, 3.59, 6.97, and 6.48 on the basis of toxicity data, and 3.23, 2.84, 6.07, and 5.27 on the basis of uptake data. The use of the alternative WHAM-Ftox approach, requiring fewer model parameters than the BLM but with similar Akaike information criterion (AIC) values, successfully predicted the toxicity and accumulation of La/Ce as well as toxicity of La-Ce mixtures, with at least 76.4% of variations explained. However, caution should be taken when using this approach to explain the uptake of La-Ce mixtures. Our results provided promising tools for delineating REMs toxicity/uptake in the presence of other toxicity-modifying factors or in mixture scenarios.