High-quality Bi4-xNdxTi3O12 (BNdT, x = 0, 0.5, 0.85) single crystals were grown by the self-flux method using Bi2O3 as a flux. Effects of Nd substitution on the structure and electric properties of the crystals were investigated. X-ray diffraction results indicate that Nd substitution leads to the orthorhombic-tetragonal transition of BNdT structure. Ferroelectric properties and leakage currents of the BNdT crystals were measured along different directions. It was found that both the polarization and the leakage currents of the BNdT single crystals decrease with increasing Nd content. Raman spectra of the crystals at room temperature suggest that their Curie temperature T-c decreases with Nd substitution, in good agreement with the results of ferroelectric measurements. (C) 2008 Elsevier B.V. All rights reserved.