Ferroelectric (Pb 0.8 ,La 0.1 ,Ca 0.1 )TiO 3 /Pb(Zr 0.2 ,Ti 0.8 )O 3 (PLCT/PZT) bilayered thin film was prepared on Pt(111)/Ti/SiO 2 /Si(100) substrate by RF magnetron sputtering technique. Pure perovskite crystalline phase, determined by X-ray diffraction, was formed in the PLCT/PZT bilayer. The bilayered film exhibited a very dense and smooth surface morphology with a uniform grain size distribution. The ferroelectric domain structures were investigated by a combination of vertical and lateral piezoresponse force microscopy (VPFM and LPFM, respectively). It is demonstrated by both VPFM and LPFM observations that out-of-plane and in-plane lamellar ferroelectric domains coexist in the bilayered thin film. The PLCT/PZT bilayered film possesses good ferroelectric properties with relatively high spontaneous polarization (2P s =82 µC/cm 2 ) and remnant polarization (2P r =26.2 µC/cm 2 ).