Highly (100) oriented Pb(Zr,Ti)O3 [PZT] films were fabricated using lanthanum nitrate/nickel acetate double layers as a buffer layer, regardless of the other deposition conditions, such as the pyrolysis temperature, pyrolysis time, annealing temperature, and heating rate. The buffer layer was also acted as a very effective barrier against Pb-Si interdiffusion, thus allowing for the direct deposition of PZT films on Si, SiO2/Si, and glass substrates. The strong orientation was attributed to the formation of a crystalline intermediate phase between the PZT and lanthanum nitrate during annealing. The lanthanum nitrate/nickel acetate double layers became a lanthanum nickel oxide (LaNiO3), which shows good electrical conductivity, after an annealing process at 650°C. The nature and the role of lanthanum nitrate buffer as a layer for the growth of highly (100) oriented PZT films have been studied. The dielectric, ferroelectric, piezoelectric and electrooptic properties of the highly (100) oriented PZT films with a lanthanum nitrate/nickel acetate buffer layer were measured and compared with the values measured from the (111) and (100) oriented PZT films deposited without buffer layer.