Dielectric properties of electrospun polyvinylpyrrolidone (PVP) and polyacrylonitrile (PAN) nanocomposite fibers were determined as a function of temperature and concentration in order to explore the possibility of using them as dielectric materials in different industrial applications. Multiwall carbon nanotubes and (NiZn ferrite) were individually dispersed into the polymeric solutions of PVP and PAN and were then electrospun at various conditions. Thin layers of films were placed between two parallel Al electrode plates of the capacitance bridge prior to the measurements. We determined that nanoscale inclusions and temperature mainly affect the dielectric properties of the nanocomposite fibers. The dielectric studies can provide critical information for many electronic applications, such as loss of a cable insulator, the impedance of a substrate, and the frequency of a dielectric resonator.