A comprehensive study of the magnetic behavior, morphology, and composition of Fe-containing oxide coatings on aluminum and titanium has been carried out to investigate the origin of their ferromagnetism. The coatings have been formed by the plasma electrolytic oxidation (PEO) technique in slurry electrolytes containing colloidal particles of iron(III) hydroxides. On the surface of coatings on Al, iron is distributed unevenly concentrating in defective areas with a large number of small pores, and near large pores. On the surface of coatings on Ti, iron and titanium are distributed in antiphase in areas of comparable size. Within the pores, iron concentration appears about 5–10 times higher and oxygen concentration 3–4 times lower than their average concentration over the surface. In both cases, localization of the areas with ferromagnetic properties follows the peculiarities of iron distribution on the surface. The magnetic fraction in the coatings on aluminum appears to be represented by iron-aluminum spinel Fe_3-xAl_xO₄ with x > 0.06, likely cation-deficient. Elemental iron and traces of iron hydroxides are also possibly present. In the coatings on titanium, titanomagnetite (Fe_3-xTi_xO₄, where x ∼ 0.2–0.3) or its oxidized analogue, titanomaghemite, appear to be present, and possibly also some Fe–Ti alloy particles.