In this study, we demonstrate the electric and magnetic manipulation of nanoscale M-type Barium Hexaferrite (nBF) in polydimethylsiloxane (PDMS) to engineer a multifunctional nanocomposite with improved dielectric and magnetic properties. First, we synthesized the single crystal nBF via the hydrothermal synthesis route. The hydrothermal temperature, duration, and surfactant conditions were optimized to improve the magnetic properties of the nBFs, with further improvement achieved by post-annealing. The annealed nBFs were aligned dielectrophoretically (DEP) in the polymer matrices by applying an AC electric field. Under the influence of this electric field, nBFs were observed to rotate, align and form chains within the polymer matrix. Optical microscopy (OM) imaging was used to determine the electrical alignment conditions (duration, magnitude, and frequency) and these parameters were used to fabricate the composites. A Teflon setup with Indium Tin Oxide (ITO) coated Polyethylene Terephthalate (PET) was used, where the ITO coatings act as electrodes for the electric field-manipulation. To simultaneously apply the magnetic field, this Teflon setup is placed between two permanent magnets capable of generating a 0.6 T external magnetic field. Along with electric and magnetic fields, concurrent heating was applied to cure the PDMS and freeze the microstructure formed due to electric and magnetic fields. Upon completion of the curing step, parallel chain formation is observed under OM. The X-Ray Diffraction(XRD) results also confirm that the particles are magnetically oriented in the direction of the magnetic field within the chain. Vibrating Sample Magnetometry (VSM) measurements and dielectric spectroscopy are used to characterize the extent of anisotropy and improvement in dielectric and magnetic properties compared to random composites. We find that simultaneous electric and magnetic field alignment improves the dielectric properties by 12% compared to just magnetic alignment. We also observe 19% improved squareness ratio when both fields are applied. The possibility of simultaneous electrical and magnetic alignment of magnetic nanoparticles will open up new doors to manipulate and design particle-modified polymers for various applications.