The dielectric properties and tunability of multilayer thin films with compositional PbZr0.52Ti0.48O3/Bi1.5Zn1.0Nb1.5O7 (PZT/BZN) layers (PPBLs) fabricated by pulsed laser deposition on Pt/TiO2/SiO2/Si substrate have been investigated. Dielectric measurements indicate that the PZT/BZN bilayer thin films exhibit medium dielectric constant of about 490, low loss tangent of 0.017, and superior tunable dielectric properties (tunability=49.7% at 500 kV/cm) at a PZT/BZN thickness ratio of 3, while the largest figure of merit is obtained as 51.8. The thickness effect is discussed with a series connection model of bilayer capacitors, and the calculated dielectric constant and loss tangent are obtained. Furthermore, five kinds of thin-film samples comprising single bilayers, two, three, four and five PPBLs were also elaborated with the final same thickness. The four PPBLs show the largest dielectric constant of ~538 and tunability of 53.3% at a maximum applied bias field of 500 kV/cm and the lowest loss tangent of ~0.015, while the largest figure of merit is 65.6. The results indicate that four PPBLs are excellent candidates for applications of tunable devices.