ABSTRACT Natural-superlattice-structured Bi2MoO6−Bi4Ti3O12 (BM-BIT) (m = 1–3) thin films have been prepared on Pt/TiO2/SiO2/Si and SrTiO3 (001) single crystal substrates by pulsed laser deposition and show very good ferroelectric properties. The BM-BIT film seems to be almost single phase and its c-lattice constant is estimated to be 2.47 nm. This lattice constant is very close to that (2.45 nm) of the superlattice structure consisting of one BM unit cell and one BIT unit cell, namely 1-1 superlattice of BM-BIT. This natural-superlattice structure consisting of non-sequential m number BLSF materials such as m = 1–3 has never been reported so far. Polycrystalline BM-BIT (m = 1–3) thin film on Pt/TiO2/SiO2/Si substrate deposited at 450°C and post-annealed at 650°C has large remanent polarization (2P r = 54 μC/cm2) and the P-E hysteresis loops show good saturation behavior for the applied field.