We demonstrate the fabrication of free-standing polymeric nanocomposite films, which present magnetic and electrically conductive anisotropic properties. Magnetically functionalized carbon nanofibers are dispersed in a polymeric solution and, upon casting under a weak external magnetic field, are easily oriented and permanently assembled in a head-to-tail orientation in the polymer film during solvent evaporation. Magnetic and conductive property studies reveal that the resulting films have a high degree of anisotropy in both cases, thus allowing their use in functional complex devices. As a proof of concept, we demonstrate the potential application of these films as flexible THz polarizers. The detailed study shows that very high attenuation values per unit film thickness and fiber mass concentration are achieved, paving thus the way for cost-effective fabrication of substrate-free systems that have advantage over conventional devices realized so far.