Cyanoethyl cellulose (CYC) possesses a unique property of high dielectric constant (ε = 35–38). Highly substituted CYC also exhibits high water resistance, high insulation, and self-extinguishing properties, along with good liquid crystal behavior. CYC can be used as an electroluminescent material and is one of the best materials for developing large-screen television transmitters, new radar fluorescent screens, and small laser capacitors in optical weapon systems. It is mainly used as the primary dielectric in high-dielectric coatings and high-dielectric thin-film capacitors. It is also used as an electroluminescent material in special light sources, as a dielectric in military plastic flexible lamps, and as a high-dielectric plastic sleeve in reconnaissance radar. This research aims to prepare a CYC based high-dielectric flexible nanocomposite film, providing a CYC based high-dielectric flexible nanocomposite film with high dielectric constant, low dielectric loss, good mechanical properties, and thermal stability, as well as its preparation method. A CYC based high-dielectric flexible nanocomposite film is prepared by using CYC as the matrix, ceramic fillers, and conductive fillers as auxiliary materials, forming a solution, and then casting it into a film.