Ferroelectric Bi4Ti3O12 thin films have been deposited using second harmonics of a Q-switched Nd:YAG laser. Various single crystal substrates, including SrTiO3(100), SrTiO3(110). MgO(100), and MgO(110), were used. Structural and electro-optic properties of the films were investigated using XRD, x-ray pole figure, and linear birefringence measurements. It is found that substrate kinds and their surface orientations are important growth parameters which determine crystal axis orientation and electro-optic properties of the Bi4Ti3O12 thin films.