Single phase polycrystalline Nd-modified BNFNT-x series 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 FeO₆, nor NiO₆ nor TiO₆. 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 (2P_r) of ～ 19.7 $ \mu {\rm C/cm }^2$. The room-temperature magnetization (2M_s) can reach a maximal value of ～ 4.132 emu/g (1 emu/g = 10 ³ A·m²/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 Fe³⁺ and Fe²⁺. The room-temperature magnetization (2M_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 Fe³⁺—O—Fe³⁺, Fe³⁺—O—Ni³⁺ and Ni³⁺—O—Ni³⁺, 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.