systems, they have numerous applications in various fields as pulsed power supply technology, [8,9] energy harvesting, [10][11][12] inverters, [13][14][15] and passive elements, [16][17][18] toward both defense and civil industries. Excellent energy storage capabilities of dielectric materials including high discharged energy density and high energy efficiency have long been eagerly pursued to meet the challenges and needs of the rapid development of modern industry, i.e., the low energy density of current dielectric materials results in overburdened capacitor volume and weight in electrical power systems. The energy storage performances of dielectric materials are usually multiply determined by three major electrical and dielectric parameters, which are categorized as:1) The breakdown strength E b ;2) The relative permittivity (also called dielectric constant) ε r or electric displacement D (the electric displacement is related to the polarization P by D = P + ε 0 E, here ε 0 = 8.85 × 10 −12 F m −1 is the vacuum permittivity); 3) The dielectric loss tanδ.In general, as illustrated in Figure 1, the discharged energy density of dielectric materials can be determined aswhere E is the applied electric field, and the energy efficiency is calculated by Dielectric polymer nanocomposites by integration of high-E b polymer matrix and high-D(ε r ) ceramic fillers have shown great potential for dielectric and energy storage applications in modern electronic and electrical systems. Interface between ceramic fillers and polymer matrix is considered as a predominant factor to determine the dielectric performances of the nanocomposites. This review analyzes the influence of the interface on dielectric responses and breakdown strength in the nanocomposites, and discusses the viability of current interface engineering strategies in improving their energy storage capabilities. Two scopes of current interface modification approaches are focused from both structural and functional considerations in the dielectric ceramics/polymer nanocomposites: first, the organic/inorganic interface compatibility can be modified to generate homogeneous dispersion of ceramic nanoparticles in polymer matrix, which is the premise of fully realizing the synergistic combination of advantages of polymer and ceramic fillers; second, regulated local electrical and dielectric behaviors in interface region enable the enhancement of dielectric properties (both high dielectric constant and high breakdown strength) in resultant nanocomposites. In the last part, some present challenges and future perspectives are proposed to utilize the interface strategy for developing high energy density ceramics/ polymer nanocomposites for dielectric and energy storage applications.