“Core/shell” composites are based on a ferrite core coated by two layers with different properties, one of them is an isolator, SiO2, and the other is a semiconductor, TiO2. These composites are attracting interest because of their structure, photocatalytic activity, and magnetic properties. Nanocomposites of the “core/shell” МFe2O4/SiO2/TiO2 (М = Zn(II), Co(II)) type are synthesized with a core of MFe2O4 produced by two different methods, namely the sol-gel method (SG) using propylene oxide as a gelling agent and the hydrothermal method (HT). SiO2 and TiO2 layer coating is performed by means of tetraethylorthosilicate, TEOS, Ti(IV) tetrabutoxide, and Ti(OBu)4, respectively. A combination of different experimental techniques is required to prove the structure and phase composition, such as XRD, UV-Vis, TEM with EDS, photoluminescence, and XPS. By Rietveld analysis of the XRD data unit cell parameters, the crystallite size and weight fraction of the polymorphs anatase and rutile of the shell TiO2 and of the ferrite core are determined. The magnetic properties of the samples, and their activity for the photodegradation of the synthetic industrial dyes Malachite Green and Rhodamine B are measured in model water solutions under UV light irradiation and simulated solar irradiation. The influence of the water matrix on the photocatalytic activity is determined using artificial seawater in addition to ultrapure water. The rate constants of the photocatalytic process are obtained along with the reaction mechanism, established using radical scavengers where the role of the radicals is elucidated.