Lead-free films of Bi4-xNdxTi3O12 were deposited on Pt(111)/Ti/SiO2/Si(100) substrate via spin-coating methods. It is shown that there are no secondary phases in Bi4-xNdxTi3O12 films and clear interfaces between the Bi4-xNdxTi3O12 films and substrates when the films are annealed at 700 ℃. And the Bi4-xNdxTi3O12 films also exhibit a blue light emission peak at 437 nm and a yellow light emission peak at 580 nm. There are narrower band gaps, higher dielectric constant and lower dielectric loss when Nd3+ concentration varies from 0 to 0.85. And the Bi3.15Nd0.85Ti3O12 film possesses the minimum of band gap energy (2.67 eV). Moreover, Bi3.55Nd0.45Ti3O12 film exhibits a minimal leakage current density and a maximal remanent polarization, which is highly beneficial for the potential applications in multi-functional devices.