Bi3.7Nd0.3Ti3O12 (BNT0.3) films were fabricated on indium tin oxide/glass substrates using a metal organic decomposition method at temperatures ranging from 500 degrees to 650 degrees C. A predominantly (100)-oriented BNT0.3 film can be obtained even at 550 degrees C. The growth mode of the predominantly (100)-oriented BNT0.3 films fabricated by the sequential layer annealing method was discussed based on the structure evolution with the annealing temperature and the film thickness. The largest values of the remanent polarization and piezoresponse are observed in the BNT0.3 film annealed at 650 degrees C, which can be ascribed to the grain growth and the release of the in-plane residue tension stress.