The paper investigates the possibility of fabricating a carbon nanotubes (CNT)-modified nanocomposite based on pyrolyzed polyacrylonitrile (PPAN). The layered structure of PPAN ensures the attachment of nanotubes (NT) to the polymer matrix, forming enhanced PPAN/CNT nanocomposites. We synthesized a PPAN/CNT polymer nanocomposite and investigated its mechanical, conductive, and electronic properties. Using the quantum chemical method density functional theory (DFT), we studied an interaction mechanism between PPAN and single-walled carbon nanotubes. We described the structural features and electron energy structure of the obtained systems. We found that the attachment of a CNT to the PPAN matrix increases tensile strength, electrical conductivity, and thermal stability in the complex. The obtained materials were exposed to electromagnetic radiation and the dielectric constant, reflection, transmission, and absorption coefficients were measured. The study demonstrates the possibility of using carbon nanotubes for reinforcing polyacrylonitrile polymer matrix, which can result in the development of an enhanced class of materials possessing the properties of both polymers and CNTs.