Magnetic, magnetic resonance, and structural properties of iron and cobalt nanoparticles embedded in a polyethylene matrix were studied. The materials were prepared by thermal decomposition of cobalt or iron formate in a polyethylene melt in mineral oil and contained from 2 to 40% wt. of metal. Transmission electron microscopy data indicate that the average diameter of particles is up to 8.0 nm. According to extended x-ray absorption fine structure and Mössbauer spectroscopy studies, the particles comprise a metallic core and nonmetallic shell which is chemically bound to the surrounding matrix. Electrophysical and magnetic properties of the materials prepared were studied along with their reflection and attenuation factors in the super high frequency band. The materials were found to be suitable for use in electromagnetic shielding.