Based upon the dielectric and magnetic properties of perovskite and U-type hexaferrite, composite of these materials have been selected for this study. The composites, (1-x)PNT-x(Sr1-3xNd2x)4Co2Fe36O60 where x = 0.42, 0.44, 0.46, 0.48 are manufactured using the solid state reaction process. and analyzed for phase formation. The magnetic, dielectric and magneto-dielectric properties have been considered. The coupling between the electric and magnetic domains on imposing electric and magnetic forces on the materials has been established under this work. All of the samples showed magneto-electric coupling, according to the magneto-dielectric investigation. The sample, however, indicates the highest coupling for x = 0.46 with MDR% values of 90.68% which may be due to the appearance of high magneto-resistance (68.23%) in this sample.