The Pb(Zr 0.20 Ti 0.80 )O 3 /(Pb 1− x La x )Ti 1− x /4 O 3 (x=0, 0.10, 0.15, 0.20) (PZT/PLT x ) multilayered thin films were in situ deposited on the Pt(111)/Ti/SiO 2 /Si(100) substrates by RF magnetron sputtering technique with a PbO x buffer layer. With this method, all PZT/PLT x multilayered thin films possess highly (100) orientation. The PbO x buffer layer leads to the (100) orientation of the multilayered thin films. The effect of the La content in PLT x layers on the dielectric and ferroelectric properties of the PZT multilayered thin films was systematically investigated. The enhanced dielectric and ferroelectric properties are observed in the PZT/PLT x (x=0.15) multilayered thin films. The dielectric constant reaches maximum value of 365 at 1KHz for x=0.15 with a low loss tangent of 0.0301. Along with enhanced dielectric properties, the multilayered thin films also exhibit large remnant polarization value of 2P r =76.5μC/cm 2 , and low coercive field of 2E c = 238KV/cm.