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Multiferroic composites consisting of a single-phase multiferroic [0.6(PbZr0.53Ti0.47O3)-0.4(PbFe0.5Ta0.5)O3] as a matrix and a magnetostrictive phase (Co0.6Zn0.4Fe1.7Mn0.3O4) dispersed in the matrix are fabricated via hybrid synthesis technique. The structure and surface morphology studies using x-ray diffraction and field emission scanning electron microscopy techniques indicate the formation of 3-0 type particulate composites. Coexistence of soft-magnetic behavior and ferroelectric characteristics are confirmed for composites from magnetization vs magnetic field (M–H) and polarization vs electric field (P–E) measurements, respectively. Magneto-dielectric (MD) measurement shows significant changes in the dielectric properties with the application of a magnetic field, indicating the existence of strong MD behavior. The biquadratic nature of magneto-electric (ME) coupling is described by the Landau free energy equation arising from the strain transfer at the interfaces between the constituent phases. The direct magneto-electric voltage coefficient measurement also confirms very strong coupling between ferroelectricity and magnetism and supports the strain-mediated magneto-electric effect in composites. The Φ = 0.3 composite exhibits the maximum ME coefficient of 20.72 mV/cm Oe with MS = 24.62 emu/g, HC = 59.66 Oe, and piezoelectric coefficient value d33 = 19 pC/N. The strong magneto-electric effect along with low dielectric loss at room temperature in these composites suggests their suitability for multifunctional magneto-electric device applications such as magnetic sensors, etc. [ABSTRACT FROM AUTHOR]