The magnesium-zinc ferrites MgZnFeO (x = 0…1) were studied as magnetic sorbents for environmental applications. Low-temperature Mössbauer spectroscopy was used to determine the distribution of magnesium and ferric ions in the spinel crystal lattice. The influence of Zn content on magnetic parameters was investigated on the basis of VSM data. As the molar ratio of zinc to magnesium increases from 0 to 1, the pH value decreases from 10.5 to 8.9. Langmuir and Freundlich models were used to check whether single-layer or multi-layer adsorption occurs. The adsorption of Cr(VI) and Ni(II) ions is well fitted by the Langmuir equation. To check the physical or chemical nature of the sorption process, the Dubinin-Radushkevich equation was used. It was found that the processes of adsorption of Cr(VI) and Ni(II) ions are of a chemical nature. The best Cr(VI) ion adsorption capacity was found for the MgZnFeO sample (q = 30.49 mg/g). The percentage of heavy metal removal by the mixed ferrite samples increases with increasing zinc content. The most effective sorbent for Ni(II) removal is the MgZnFeO sample (93.2%). Modeling the antistructure provides deeper insight into the mechanism of heavy metal adsorption. The obtained magnesium-zinc ferrites are promising magnetic adsorbents for removing chromate and nickel ions from the environment.