0.9Bi1 − xNdxFeO3 – 0.1PbTiO3 solid solution where x = 0.05, 0.10, 0.15 and 0.20 were success fully synthesized by the standard solid-state reaction method. The effect of Nd3+ion substitution on structural, micro structural, ferroelectric, magnetic, dielectric and magneto-electric properties of 0.9BiFeO3-0.1PbTiO3 have been investigated. The XRD analysis for the samples under study revealed distorted rhombohedral structure with R3C space group. 0.9Bi1 − xNdxFeO3 – 0.1PbTiO3 where x = 0.05, 0.10, 0.15 and 0.20 i.e.(BNFPT)x compounds crystallised as single-phase materials with the same structure as the parent BiFeO3 compound.. The SEM study revealed the uniform grain scattering for all prepared samples. Raman spectroscopy showed disappearance of some Raman modes indicated a structural phase transition with substitution of Nd dopants at Bi site and also confirmed the distorted rhombohedral perovskite structure of (BNFPT)x compounds with R3c symmetry. Dielectric measurements showed magnetoelectric coupling around Neel temperature in all the samples and also improved dielectric properties with addition of dopants in BiFeO3(BFO) compound. All the prepared samples exhibit weak ferro-magnetic character at room temperature. However, the variation in linear behavior and enhancement in magnetization is found at 5 K which shows gradual increase in remnant magnetization from 0.00785 emu/g to 0.37513 emu/g with increase in Nd doping for all (BNFPT)x samples. Nd doping reduces leakage current by three orders of magnitude, from 10− 4 to 10− 7. Ferroelectric study revealed the pinning effect in hysteresis loops with low remnant polarization.