The non-toxic lead-free multiferroic composite samples Ni0.7Mg0.3Fe2O4/BaZr0.2Ti0.8O3 were synthesized by using standard double sintering ceramic method. The composite samples are found to exhibit dielectric response, which might be associated with Maxwell-Wagner type interfacial polarization and Koop's phenomenological theory. The variation of DC conductivity with respect to temperature revealed the conduction of electrons i.e. due to the small polarons hopping mechanism. The synthesized ME composite samples show a representative magnetic hysteresis (M − H) loop type behaviour at room temperature. In a previous report, the response of ME voltage coefficient 4.262 mVcm-1.Oe was determined for (30%) Ni0.8Mg0.2Fe2O4 + (70%) BaZr0.2Ti0.8O3 composites at 5.0 kOe applied DC magnetic field. But in this report, we improved the ME voltage coefficient for the composition 50% (Ni0.7Mg0.3Fe2O4) + 50% (BaZr0.2Ti0.8O3) which is a lead-free ME composite with the massive ME voltage coefficient of 8.562 mV/cm.Oe was achieved. Hence, the estimated results can provide experimental guidance for the optimal design of high-performance magnetoelectric devices and render better support for the technological development in the field of magnetoelectricity.