Widespread use of pesticides has resulted in the accumulation of pesticide residues in the environment due to their persistence and stability. To reduce potential exposures, we have developed broad‐acting clay‐based sorbents that can be included in the diet as enterosorbents to reduce the bioavailability and toxicity of chemicals. In the present study, parent and acid‐processed calcium montmorillonite clays (CM and APM, respectively) were used to determine their potential as sorbents of the organochlorine insecticide dieldrin. We used adsorption isotherms, thermodynamics, and dosimetry studies to determine the capacities and affinities of the clays, the enthalpies of the binding reactions, and potential doses of sorbent that could protect against high exposures. Adsorption isotherms for APM fit a Langmuir model with high enthalpy (suggesting chemisorption) and high capacity (Qmax value = 0.45 mol kg–1), indicating tight binding of dieldrin. Cultures of Hydra vulgaris were used to determine the ability of sorbents to protect a living organism from dieldrin toxicity. The inclusion of acid‐processed clays resulted in the highest reduction of dieldrin toxicity (70%) in the hydra. Further work indicated that both CM and APM can significantly reduce the bioavailability of dieldrin from soil (p ≤ 0.01). These results suggest that APM (and similar clays) can be effective sorbents of dieldrin and may be included in the diet and/or soil to protect against environmental exposures. Environ Toxicol Chem 2020;39:517–525. © 2019 SETAC