Multiferroic BFO/PZT(5/95) multilayer films were fabricated by spin-coating method on the Pt/Ti/SiO2/Si substrate alternately using BFO and PZT(9/95) alkoxide solutions. The structural and dielectric properties were investigated with variation of the solvent and the number of coatings. All films showed the typical XRD patterns of the perovskite polycrystalline structure without presence of the second phase such as Bi2Fe4O3. BFO/PZT multilayer thin films showed the typical dielectric relaxation properties with increase an applied frequency. The average thickness of 6-coated BFO/PZT multilayer film was about 600 nm. The dielectric properties such as dielectric constant, dielectric loss and remnant polarization were superior to those of single composition BFO film, and those values for BFO/PZT multilayer film were 1199, 0.23% and 12 μC/cm2.