The preparation of hybrid films of metal (Ti and Sn) phosphate nanosheets and polyaniline by simultaneous electrophoretic and electrolytic deposition was performed in an acetonitrile solvent. Emeraldine polyaniline was intercalated between the phosphate nanosheets with a monolayer arrangement. The obtained hybrid films were several tens of micrometers in thickness. The ratio of incorporated polyaniline to metal phosphate in the hybrid films reaches to around 0.45 and 0.30 at suitable concentrations of tetrabutylammonium hydroxide (TBAOH). These amounts correspond with occupancy of polyaniline in the interlayer gallery of several tens percent. Fractions of voids in a horizontal direction were around 22 and 1% in titanium phosphate/polyaniline and tin phosphate/polyaniline hybrid films, respectively. Thus, anodic electrodeposition makes it possible to form thick films of intercalation compounds of alpha-titanium and tin phosphates with polyaniline. These hybrid films were examined for redox activity. The cyclic voltammetry results of these films confirmed that the hybrid films have redox activity by polyaniline. For these voltammograms, the maximum current was observed in the tin phosphate/polyaniline hybrid deposited for 15 min. The redox activity of these hybrids possibly depends on the mesoscopic texture of the film, especially on the amount of voids in a horizontal direction.