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Abstract Multiferroic composites are promising candidates for magnetic field sensors, next-generation low power memory and spintronic devices, as they exhibit much higher magnetoelectric (ME) coupling and coupled ordering parameters compared to the single-phase multiferroics. Hence, the 3-0 type particulate multiferroic composites having general formula (1 − Φ)[PbFe0.5Nb0.5O3]-Φ[Co0.6Zn0.4Fe1.7Mn0.3O4] (Φ = 0.0, 0.05, 0.1, 0.2, 0.3, 0.4, 0.5, 1.0, (1 − Φ) PFN-ΦCZFMO) were prepared using a hybrid synthesis technique. Preliminary structural and microstructural analysis were carried out using XRD and FESEM techniques, which suggest the formation of 3-0 type particulate composite without the presence of any impurity phases. The multiferroic behaviour of the composites is studied with polarization versus electric field (P-E) and magnetization versus magnetic field (M-H) characteristics at room temperature. The nature of ME coupling was investigated elaborately by employing the Landau free energy equation along with the magneto-capacitance measurement. This investigation suggests the existence of biquadratic nature of ME coupling (P2M2). The magneto-electric coupling measurement also suggests that strain mediated domain coupling between the ferroelectric and magnetic ordering is responsible for the magneto-electric behaviour. The obtained value of direct ME coefficient 26.78 mV/cm-Oe for Φ = 0.3, found to be higher than the well-known single-phase materials and polycrystalline composites.