Bi4Ti3O12 (BIT) thin films with TiO2 anatase layer were prepared on La0.05Sr0.95TiO3 (LSTO) substrates by metalorganic vapor deposition using Bi(CH3)3 and Ti(i-OC3H7)4 sources. When the substrate temperature was fixed at 500oC, the BIT thin films exhibited highly c-axis orientation. The c-axis orientation does not depend on layer created on LSTO substrate. The grain size of BIT thin film with TiO2 anatase layer is smaller than that with of BIT thin film with no-layer. The grain size of the BIT thin film accords with that of TiO2 anatase layer. This indicates that the TiO2 anatase layer acts not as barrier layer but as an initial nucleation layer of the BIT thin film. The postannealed BIT thin film with TiO2 anatase layer exhibited random orientation and P-E hysteresis loop.