In principle, the energy density (U) of dielectric capacitors is determined by the applied electric field (E) and the electric displacement (D) asAnd the electric displacement (D) is associated with the polarization P and dielectric constant ε r by D = P + ε r ε 0 E. For linear dielectric capacitors, U = 1/2DE = 1/2ε r ε 0 E 2 , where ε 0 is the vacuum permittivity (ε 0 = 8.85 × 10 −12 F m −1 ). Since breakdown strength E B is the utmost E that can be applied to dielectric capacitors, both ε r and E B have to be enhanced simultaneously to obtain high energy density. Ceramics show high dielectric constant but low breakdown strength; while polymers exhibit high breakdown strength but low dielectric constant. [11,12] Hence ceramics nanofillers, such as TiO 2 , [13] BaTiO 3 , [14] and Ba x Sr 1−x TiO 3 , [15] are introduced into the polymer matrix to form polymer nanocomposites in order to compensate for each other's deficiencies. Unfortunately, previous studies have suggested that improved ε r of polymer nanocomposites is obtained merely at the expense of breakdown strength. [13] Thus, it is impracticable to effectively increase both parameters in the polymer nanocomposites.It has been widely demonstrated that interfacial polarization is the primary mechanism of polarization in polymer nanocomposites, caused by the large contrast in the dielectric constant and conductivity at the interface between the polymer matrix and fillers. [16][17][18][19] The high E B and large U of nanocomposites may be attributed to a small leakage current, low dielectric loss, and low interfacial polarization. [20] After years of intensive study, novel strategies have been proposed to resolve the seeming paradox of enhancing ε r while maintaining high E B . One method for modulating the polymer-filler interface is surface functionalization of ceramic fillers with surfactant or oligomers, [21][22][23] which can suppress filler aggregation and retard the movement of charge carriers in the surface between the polymer matrix and fillers. Perry and co-workers reported that phosphonic acid surface modifiers improve the dispersion of BaTiO 3 nanoparticles in nanocomposite films, which lead to high ε r and high E B . [24] Another universal way to alleviate the interfacial polarization between the filler and the polymer matrix is to employ core-shell structured nanofiller. [25][26][27][28] A recent study by Wang and co-workers revealed that 2D hexagonal boron nitride nanosheets and BaTiO 3 nanoparticles, used to improve E B and The dielectric capacitor with high electric energy density is demanded for modern electronic and electrical power systems. However, their energy density is considerably limited by a low dielectric constant and low breakdown strength. Here, thin flexible polymer nanocomposites with high energy density are obtained by only adding a small loading of 2D monolayer titania along with concurrent improvements of dielectric constant and breakdown strength. This work not only first reveals that monolayer titania is an excellent filler...