With the rapid development of power energy, electronic information, rail transit, and aerospace industries, nanocomposite dielectric materials have been widely used as new materials. Polymer/inorganic nanocomposite dielectric materials possess excellent physical and mechanical properties. In addition, numerous unique properties such as electricity, thermal, sound, light, and magnetic properties are exhibited by these materials. First, the macroscopic quantum tunneling effect, small-size effect, surface effect, and quantum-size effect of nanoparticles are introduced. There are a few anomalous changes in the physical and chemical properties of the matrix, which are caused by these effects. Second, the interaction mechanism between the nanoparticles and polymer matrix is introduced. These include infiltration adsorption theory, chemical bonding, diffusion theory, electrostatic theory, mechanical connection theory, deformation layer theory, and physical adsorption theory. The mechanism of action of the interface on the dielectric properties of the composites is summarized. These are the interface trap effect, interface barrier effect, and homogenization field strength effect. In addition, different interfacial structure models were used to analyze the specific properties of nanocomposite dielectric materials. Finally, the research status of the dielectric properties of nanocomposite dielectric materials is introduced.