Two-dimensional (2D) nanofillers can effectively improve the performance of nano-dielectrics by having larger aspect ratios and larger electron-scattering interfaces than one-dimensional (1D) nanofillers and zero-dimensional (0D) nanofillers; the formation of a large interfacial area in the polymer matrix effectively traps or scatters the mobile charges and increases the curvature of the propagation paths of the electric tree, thus effectively increasing the breakdown strength and the energy-storage density of nanodielectrics. In this article, the intrinsic mechanism of 2D nanodielectrics is elaborated using percolation theory, microcapacitance theory, interfacial model, and ping-pong racket model. Surface modification, oriented alignment, and multilayer structural design are reviewed to enhance the dielectric properties of nanodielectrics. Additionally, an outlook on the multiple challenges and potential opportunities in the process of preparing energy-storage capacitors with excellent performance is provided. The two-dimensional (2D) nanosheets can significantly block the propagation path of electrical trees, extend the breakdown path of the material, and thereby effectively enhance the breakdown strength and service life of the nano-dielectric. Meanwhile, these parallel-arranged nanosheets can also form microcapacitor structures, greatly enhancing the dielectric constant and energy-storage performance of the nano-dielectric.image (c) 2024 WILEY-VCH GmbH