Ferrite (Ni0.6Co0.4Fe2O4) phase, ferroelectric (Pb(Mg1/3Nb2/3)(0.67)Ti0.33O3) phase and magnetoelectric composites of (x)Ni0.6Co0.4Fe2O4 + (1 - x)Pb(Mg1/3Nb2/3)(0.67)Ti0.33O3 with x = 0.15, 0.30 and 0.45 were prepared using solid-state reaction technique. Presence of Ni0.6Co0.4Fe2O4 and Pb(Mg1/3Nb2/3)(0.67)Ti0.33O3 was confirmed using X-ray diffraction technique. The scanning electron microscopic images were used to study the microstructure of the composites. Connectivity scheme present in the magnetoelectric (ME) composites are discussed from the microscopic images. Variation of dielectric constant and dielectric loss with temperature for all the Composites Was Studied. Here we report the effect of Ni0.6Co0.4Fe2O4 mole fraction on connectivity schemes between Ni0.6Co0.4Fe2O4 and Pb(Mg1/3Nb2/3)(0.67)Ti0.33O3 composite. The variation of magnetoelectric voltage coefficient with dc magnetic field shows peak behaviour. The Maximum value of magnetoelectric voltage coefficient of 9.47 mV/cm Oe was obtained for 0.15Ni(0.6)Co(0.4)Fe(2)O(4) + 0.85Pb(Mg1/3Nb2/3)(0.67)Ti0.33O3 composites, Finally we have co-related the effect of Ni0.6Co0.4Fe2O4 content and dielectric properties on magnetoelectric voltage coefficient. (C) 2009 Elsevier Ltd. All rights reserved.