Fullerene films of controlled surface topography were prepared by electrophoretic deposition from toluene-ethanol mixed solvent solutions. The AFM imaging of the films revealed that the size of the C₆₀ grains in films could be readily controlled both with the time of C₆₀ aggregation in bulk solution before the deposition and strength of the applied dc electric field. The film deposition was monitored by piezoelectric microgravimetry with the use of an electrochemical quartz crystal microbalance. The mass of the C₆₀ film increased exponentially with the time of deposition. The corresponding decrease of the deposition rate with time was presumably due either to the growth of larger C₆₀ aggregates in solution of lower mobility or blocking effect of the electrode surface by insulating C₆₀ deposits. In the accessible potential window of 0.1 M (TBA)PF₆, in acetonitrile, cyclic voltammetry curves for the C₆₀ films featured four cathodic peaks corresponding to four one-electron reductions. Simultaneously recorded multi-scan curves of current, resonant frequency change, and dynamic resistance change vs. potential for a potential range covering the first two electro-reductions (that is the range in which the film was relatively stable with respect to dissolution) indicated pronounced transformations in the film caused by the solvent-assisted dynamic equilibria of ions of the supporting electrolyte. The related to C₆₀ charge in films piezoelectric microgravimetry, XPS, and XRD analyses indicated reversible ingress of both TBA⁺ counter- and PF₆^‑ co-ion into the C₆₀^- film.