An energy efficient move toward the regulation of magnetization vector solely with E-field by developing multiferroic (MF) magnetoelectric (ME) nanostructures' have opened up vast avenues for novel low power consumption memories and magnetoelectric devices. The present study delineates the development of multiferroic nanocomposites (MF NCs) with perovskite BiFeO3 and spinel NiFe2O4. A simple Pechini one-pot method is employed for the preparation of nanocomposites with different molar concentrations and the modified structural, magnetic, dielectric, and magnetoelectric performance of NCs is carried out at room temperature. The purity in the crystalline phase of BiFeO3 and NiFe2O4 in the NCs are corroborated by XRD and FTIR spectroscopy, which is further substantiated, while EDAX analysis pointed out the elemental composition. The SEM images provide an evidence for the closely compacted and agglomerated grains with some voids in the prepared sample. A well saturated magnetic hysteresis (M–H) loop reveals long range ferromagnetic ordering and the remanence value ascertains the multidomain structure. The dielectric performance and impedance analysis imparts greater knowledge of the dependence of grain and grain boundaries on the resistive and conductive behavior of the composites. The frequency dependence of electric modulus and impedance exhibits a non-Debye type of relaxation process. The P–E hysteresis loops clearly show the lossy behavior of the composites with an increase in the NiFe2O4 concentration. The ME coupling coefficient of the composites evaluated using the dynamic magnetic field method demonstrates the effective coupling interaction between ferroelectric (FE) perovskite BiFeO3 and ferromagnetic (FM) spinel NiFe2O4. Thus, the findings disclose a greater potential for innovative applications in spintronics and information technology.