We have successfully fabricated barium titanate (BaTiO 3 ) films on Si (100) and Pt(111)/Ti/SiO 2 /Si substrates using the polyol thermal decomposition (PTD) process by spin-coating technique. In PTD process, we confirmed that the crystalline oxycarbonate Ba 2 Ti 2 O 5 CO 3 films were directly formed as a consequence of evaporation of polyol precursor solution prepared simply by mixing metal chlorides and ethylene glycol, and then converting them into crystalline BaTiO 3 films through thermal decomposition at [500°C. This feature makes it possible to grow densely packed and crack-free BaTiO 3 films as thin as 70 Å per cycle. Although PTD is described here for a complex metal-oxide film of BaTiO 3 , other simple and complex metal-oxide thin films with high-dielectric constant materials are also likely to be suitable for deposition with accurate control of film thickness and composition using the polyol precursor solutions.Metal-oxide thin films, such as AO and ABO 3 , are important components in a wide array of electronic and optical devices, and their study and manufacture involve major aspects of current science and technology [1]. The ability to deposit and tailor reliable metal-oxide films (with a particular recent emphasis on ultrathin systems) is indispensable for contemporary solid-state electronics. Many different methods are used to make these thin films, such as various physical and chemical vapor depositions mainly dependent on vacuum deposition techniques, and many new techniques have been developed [1][2][3]. However, the use of these vacuum deposition techniques, the high cost of necessary equipment, and restriction of coatings on a relatively small area have limited their potential applications [4]. On the other hand, chemical solution depositions (CSD) such as sol-gel and metallo-organic decomposition (MOD) are more cost-effective, but many metal oxides cannot be deposited, and the control of stoichiometry is not always possible owing to differences in chemical reactivity among the metals [5]. In particular, precise control of film thickness, crystallinity, and morphology are significant problems to be overcome in CSD [6].One of the challenges in solution-based processes of complex metal-oxide films has been to produce high-quality films with desired chemical composition. The sol-gel method among the CSD processes is one of the most important approaches, which are being extensively used for the fabrication of complex oxide thin films. The sol-gel method show attractive advantages due to the fact that films with extremely uniform composition over large areas can be obtained from chemical solution deposition [7]. A key issue of any CSD thin films processing is the chemistry of precursor solution, which governs the properties of the final oxide layer. Even more challenging for sol-gel processing of complex metal-oxides is the identification of a solvent system in which the multiple organometallic precursors are reciprocally compatible. Recently, a few attempts have been reportedly made to ad...