Polyvinylidene fluoride (PVDF) is an advanced functional polymer which exhibits excellent chemical and thermal stability, and good mechanical, piezoelectric and ferroelectic properties. This work opens a new strategy for the fabrication of nanocomposites, combining the functional properties of PVDF and advanced inorganic nanomaterials. Electrophoretic deposition (EPD) has been developed for the fabrication of films containing PVDF and nanoparticles of TiO2, MnO2 and NiFe2O4. An important finding was the feasibility of EPD of electrically neutral PVDF and inorganic nanoparticles using caffeic acid (CA) and catechol violet (CV) as co-dispersants. The experiments revealed strong adsorption of CA and CV on PVDF and inorganic nanoparticles, which involved different mechanisms and facilitated particle dispersion, charging and deposition. The analysis of the deposition yield data, chemical structure of the dispersants and the microstructure and composition of the films provided an insight into the adsorption and dispersion mechanisms and the influence of deposition conditions on the deposition rate, film microstructure and composition. PVDF films provided the corrosion protection of stainless steel. Overcoming the limitations of other techniques, this investigation demonstrates a conceptually new approach for the fabrication of PVDF-NiFe2O4 films, which showed superparamagnetic properties. The approach developed in this investigation offers versatile strategies for the EPD of advanced organic-inorganic nanocomposites.