Nickel-substituted Bi4Ti3O12 (i.e., Bi4-xNixTi3O12) were synthesized by sol-gel process for different compositions. Thin films were deposited on Pt (i.e., Pt/TiO2/SiO2/Si) substrate by spin coating. Materials were characterized by x-ray diffraction and Raman spectroscopy. This study indicates that the material makes a solid solution for the compositions: x = 0.00, 0.05, 0.10, 0.15, 0.20, and 0.30, where a Ni ion replaces the Bi site. The prominent effect of Ni substitution was observed in low-frequency Raman modes. Sol-gel derived thin films of Bi4-xNixTi3O12 on a Pt substrate and post annealed at 700°C were tested for ferroelectric response which showed high remnant polarization (Pr = 22 μC/cm2 for x = 0.15). The leakage current (less then 10−7 A/cm2) at low field was observed in the film with composition x = 0.15 .The polarization of the BNiT (x = 0.15) film decreased to 83% of the initial value after 1×109 switching cycles These results indicate the potential application of Ni substituted bismuth titanate films in non-volatile ferroelectric memories.