Single phase polycrystalline Nd-modified BNFNT- xseries samples are obtained from the precursors of the same chemical formula, and prepared by using the citric acid-nitrate method. The X-ray photoelectron spectroscopy measurement indicates that a slight Nd modification does not exert significant influence on the stability of the octahedral FeO ₆, nor NiO ₆nor TiO ₆. When the molar concentration of Nd exceeds 0.25, the stability of BiO layer is cemented and conducive to the insulating role of BiO layer. It is seen that a small quantity of Nd substitution for bismuth can improve the ferroelectric polarization (2 P _r) of ～ 19.7 $ \mu {\rm C/cm }^2$ . The room-temperature magnetization (2 M _s) can reach a maximal value of ～ 4.132 emu/g (1 emu/g = 10 ⁻³A·m ²/g)in the BNFNT-0.20 sample. Two anomalies are observed in the temperature-dependent dielectric loss spectrum: one is situated in the temperature range from 200 K to 400 K and the other is located in the vicinity of 900 K. It is considered that the loss anomaly found near 900 K might be associated with the viscous motion of ferroelectric domain walls. In addition, the loss peak shown in a temperature range from 200 K to 400 K shifts toward the higher temperature with measuring frequency increasing, indicating the characteristics of dielectric relaxor behavior. The activation energy is evaluated to be 0.287−0.366 eV, which suggests that the relaxor is associated with the electrons transfer and hop between Fe ³⁺and Fe ²⁺. The room-temperature magnetization (2 M _s) has reached a maximal value of ～ 4.132 emu/g in the BNFNT-0.20 sample. The lattice distortion due to the introduction of Nd changes the angle of such antiferromagnetic coupling bonds as Fe ³⁺—O—Fe ³⁺, Fe ³⁺—O—Ni ³⁺and Ni ³⁺—O—Ni ³⁺, which leads the AFM spin states to break, and thus increases the magnetic properties. While with further modification of Nd, the drastic lattice distortion reduces the occupation of the B-sites of the magnetic ions, which might be responsible for further deteriorating the magnetic properties.