Halloysite nanotubes (HNTs) are used to fabricate dielectric capacitors attributed to their tubular architecture induced interior diffusion under external electric fields. The polar nature and large lumen space of the HNTs facilitate the free movement of holes and electrons, causing large-level polarization. The dielectric property of the HNTs can be connected with fluoropolymers so that high dielectric constant and low dielectric loss values are anticipated for the hybrid system. This chapter discusses the various fluoropolymer nanocomposites containing HNTs and their dielectric performances. The variations in the dielectric stability and response with respect to the concentration, and modifications on the HNTs are discussed in detail. At the same time, different kinds of fluoropolymers and their responses are also explained for capacitor applications. Efficient and flexible HNT polymer nanocomposites are promising materials for energy storage applications.