Neodymium-modified Bi 4 Ti 3 O 12 , (Bi,Nd) 4 Ti 3 O 12 (BNT) ferroelectric thin films have been prepared on Pt/TiO x /SiO 2 /Si substrates using metal-organic precursor solutions by the chemical solution deposition method. The BNT precursor films crystallized into the Bi layered perovskite Bi 4 Ti 3 O 12 (BIT) as a single-phase above 600 • C. The synthesized BNT films revealed a random orientation having a strong 117 reflection, whereas nonsubstituted BIT thin films exhibited a random orientation with strong 00l diffractions. Among Bi 4−x Nd x Ti 3 O 12 [x = 0.0, 0.5, 0.75, 1.0] thin films, Bi 3.25 Nd 0.75 Ti 3 O 12 thin films showed a well-saturated P-E hysteresis loop with the highest P r (22 µC/cm 2 ) and a low E c (69 kV/cm) at an applied voltage of 5 V. The Nd-substitution with the optimum amount for the Bi site in the BIT structure was effective not only for promoting the 117 preferred orientation but also for improving the microstructure and ferroelectric properties of the resultant films.