Titanium(IV) oxide is one of the most widely investigated photocatalysts. However, separation of nano-sized particulate titania might result in profitless technologies for commercial applications. Additionally, bare titania is almost inactive under the Vis range of solar spectrum due to its wide bandgap. Therefore, the present study aims to prepare novel core-interlayer-shell TiO2 magnetic photocatalysts modified with metal nanoparticles (Pt, Cu), which exhibit both photocatalytic and magnetic properties, making it easily separable within the magnetic field. Accordingly, the core-shell structure of Fe3O4@SiO2/TiO2 was obtained in water/TX100/cyclohexane microemulsion. Platinum and copper were photodeposited on four TiO2 templates and characterized by X-ray diffractometry (XRD), X-ray photoelectron spectroscopy (XPS), specific surface area (BET) measurement and diffuse refiectance spectroscopy (DR-UV/Vis). Photoactivity was studied in the reaction of phenol, acetic acid, and methanol degradation under UV/Vis irradiation, using both polychromatic and monochromatic irradiation (action spectrum analysis). The core-interlayer-shell structure of Pt and Cu modified magnetic photocatalysts was confirmed using scanning transmission electron microscopy (STEM). Magnetic photocatalysts modified with platinum and copper revealed improved photoactivity both in oxidation and reduction photocatalytic reactions, as compared to unmodified Fe3O4@SiO2/TiO2 photocatalysts. Finally, the correlation between physicochemical properties and photocatalytic activities of Fe3O4@SiO2/TiO2-Pt/Cu photocatalysts was investigated. For the first time, the effect of metals' loading on the efficiency of phenol degradation and mineralization (TOC removal), and quantum efficiency of reaction in the presence of magnetic photocatalysts were analyzed. It was found that phenol can be efficiently decomposed (ca. 100%) during 60 min of UV/Vis irradiation for the photocatalyst recovered within the magnetic field during three subsequent degradation cycles.