We are examining the behavior of a composite made of ferroelectrics with strong dielectric properties and ferrites with magnetic properties due to the rising need for materials for multipurpose devices. Many application avenues will be favored by the pairing of these materials’ individual qualities with one another. Perovskite and U-type hexaferrite composite materials have been chosen for this study based on their magnetic and dielectric properties. The composites, (1?x) PLT?x(Ba1?3xNd₂x)₄Co₂Fe36O60 where x = 0.52, 0.54, 0.56, 0.58 are prepared by solid state reaction method and phase formation was examined. Consideration has been given to the magnetic, dielectric, and magneto-dielectric properties. This work has established the link between the electric and magnetic domains while applying electric and magnetic forces to the materials. The magneto-dielectric research revealed magneto-electric coupling in all of the samples. However, the sample shows the maximum coupling for x = 0.54 with MDR% values of 93.17%, which might be because this sample appears to have a high magneto-resistance (161%).