Multifunctional polymeric nanocomposites have attracted great interest due to their significantly enhanced performance and great potential in various applications, especially in telecommunications devices, network systems, and radar technology. Engineering a composite material with effective and moderate properties by properly configuring the constituents of the magneto-dielectric materials provides greater freedom in achieving the desired functionalities. Research shows that artificial materials can significantly extend the range of material properties and provide potential for new and better performance. Designing by modeling offers an innovative way for developing advanced materials. This chapter aims to introduce an advanced computational method for characterizing magnetic and dielectric properties of functional magnetic nanoparticle-modified nanocomposites. The nanocomposite was designed using epoxy matrix dispersed with spinel structural nickel–zinc–ferrite (Ni0.5Zn0.5Fe2O4) nanoparticles. Three-dimensional finite element analysis (FEA) models were generated for characterization. The effects of shape, orientation, concentration and distribution of the nanoparticles on the magneto-dielectric properties of the nanocomposites were systematically studied by computer modeling based on FEA. The effective permittivity and effective permeability of the nanocomposites were predicted by numerical method and compared with the analytical methods, such as the Maxwell–Garnett mixing rule and Bruggeman mixing rule.