Bi4-xNdxTi3O12 (BNT) films with different Nd contents (from 0 to 1 with 0.25 intervals) are prepared by the sol-gel process. The Nd substitution effects on the preferred orientation, surface morphology, phonon modes, emission bands, andelectronic band structures of the BNT films are investigated by microscopy, Raman scattering, photoluminescence, and spectroscopic ellipsometry (SE) at room temperature. X-ray diffraction indicates that the films are polycrystalline with the pure perovskite phase. Ten Raman active modes and one silicon substrate mode can be observed. The A(1g)[Bi] at about 59 cm(-1) is unchanged whereas the B-1g and A(1g)[Ti] phonon modes shift towards higher frequencies. Photoluminescence shows that the intensities of the two peaks increase with Nd concentration except the Bi3NdTi3O12 film, due to the smallest grain size and oxygen vacancy defects. Good optical functions of the BNT films are achieved due to the SE suggesting potential applications in ferroelectric-based optoelectronic devices. (C) 2014 Elsevier Ltd. All rights reserved.