Carbonyl iron (CI) is successfully incorporated as an additive into a polystyrene (PS) matrix via a highenergy ball milling method, under an n-hexane medium with volume fractions between 1% and 5% for electromagnetic interference shielding applications by the combination of magnetic CI and an insulating PS matrix. The morphology and the dispersion of CI are investigated by field emission scanning electron microscopy, which indicates a uniform distribution of CI in the PS matrix after 2 h of milling. The thermal behavior results indicate no significant degradation of the PS when there is a slight increase in the onset temperature with the addition of CI powder, when compared to the as-received PS pellet. After milling, there are no interactions between the CI and the PS matrix, as confirmed by Fourier transformed infrared spectroscopy. In this study, the milled CI-PS powder is extruded to make filaments, and can have potential applications in the 3-D printing industry.