(1 − x)[Bi0.5Na0.5TiO3-0.07BaTiO3]-xNi0.3Cu0.08Zn0.62Fe2O4 [(1 − x)BNT-BT-xNCZF] ceramics, where x = 0.1, 0.2, 0.3, 0.4, and 0.5, were synthesized a by microwave-assisted solid-state reaction route. X-ray diffraction of the sintered ceramics showed the presence of both the ferroelectric and ferromagnetic phases, which was confirmed by surface microscopy study. Dielectric study showed a strong frequency as well as temperature dependence. Polarization versus electric field (P–E) hysteresis loop study revealed that the composite samples with x = 0.4 composition showed the highest remnant polarization. M–H loop and theoretical assessment of magnetic susceptibility (χ) showed enhancement in magnetisation as well as an χ value with the incorporation of ferrite phase in the piezoelectric matrix.