We aimed to obtain magnesium/iron (Mg/Fe)-layered double hydroxides (LDHs) nanoparticles-immobilized on waste foundry sand-a byproduct of the metal casting industry. XRD and FT-IR tests were applied to characterize the prepared sorbent. The results revealed that a new peak reflected LDHs nanoparticles. In addition, SEM-EDS mapping confirmed that the coating process was appropriate. Sorption tests for the interaction of this sorbent with an aqueous solution contaminated with Congo red dye revealed the efficacy of this material where the maximum adsorption capacity reached approximately 9127.08 mg/g. The pseudo-first-order and pseudo-second-order kinetic models helped to describe the sorption measurements, indicating that the physical and chemical forces governed the removal process.