Dielectric materials can be used to control/ store charge and electric energy, which has important potential application value for the dielectric energy storage and intelligent sensing in areas such as aerospace, electronics, and military engineering. [1,2] The dielectric materials with high dielectric permittivity (ε 0 ) and low dielectric loss (tanδ) are of great significance to national security defense and economic development. [3][4][5][6] Ceramic-based dielectric materials are widely used in electronic components in communication, military, and other related fields due to their extremely high dielectric permittivity. [7][8][9] However, the complex preparation process, high processing temperature, brittleness, and low breakdown strength of ceramics greatly limit their application range. [10] Polymers are the industrial choice of dielectric materials for charge storage applications mainly because of their high breakdown strength and excellent processability. Nevertheless, it is a great challenge that the pure polymers always have a very low dielectric permittivity. [11][12][13] Therefore, the high dielectric composite materials obtained by integrating high dielectric particles and polymers in a certain physical/chemical way have great application prospects. One common approach is to add ceramic fillers such as barium titanate (BaTiO 3 ), barium strontium titanate (Ba x Sr 1-x TiO 3 ), and calcium copper titanate (CaCu 3 Ti 4 O 12 ) to the polymers to improve their dielectric properties. [14][15][16][17] However, a higher dielectric permittivity usually requires a higher loading of ceramic filler, which affects the machinability and mechanical strength of the composites. Another approach is to add conductive fillers such as Cu, Ag, graphene, and carbon nanotubes (CNTs) to the polymers, which can obtain very high dielectric permittivity at a low conductive filler loading. [18][19][20][21][22][23] Unfortunately, the conductive fillers are prone to agglomerate, resulting in excessive leakage current, which will cause the sharp increase in dielectric loss of the conductive filler/polymer composites. In recent years, researchers have been keen to combine