Using the reactive ionized cluster beam method, ferroelectric Bi4Ti3O12 is deposited at a low temperature. This method utilizes ionized and accelerated Bi and Ti clusters. Under optimum conditions, c‐axis oriented films can be formed on quartz and on Si(100) substrates at 200 and 250 °C, respectively. The crystal orientation can be controlled without changing the substrate material and temperature. Furthermore, it is found that the ionization and acceleration conditions of the Bi and Ti elements are responsible, respectively, for the BIT formation and its orientation. The dielectric constant of the films is 135 at 100 kHz and the spontaneous polarization is 4.2 μC/cm2. These ferroelectric properties are almost identical to the bulk material.