Dielectric materials can store and release electrical energy quickly and efficiently and have potential applications in the fields of rail transportation, air and space detection, and electromagnetic weapons. However, the most promising dielectric polymer composites under research suffer either from unsatisfactory energy density (U e ) or from increasing the U e at the cost of energy efficiency (η). Herein, by the solution casting method, a nanocomposite film is fabricated by introducing trace selfassembly phase-transitioned lysozyme (PTL) modified boron nitride nanosheets (mBNNS) into a blend matrix consisting of poly(vinylidene fluoride−hexafluoropropylene) P(VDF−HFP) and poly(methyl methacrylate) (PMMA). The results suggest that PTL helps improve the interfacial compatibility of the corresponding nanocomposites via hydrogen-bonding interaction effectively. The nanocomposite film with 5 wt % mBNNS shows remarkably enhanced breakdown strength (E b ) of ∼500 MV/m and U e of 14.9 J/cm 3 , which are 166% and 244% of the blend matrix, respectively. Meanwhile, η of the nanocomposite film reaches ∼71% because of the clipping effect of linear PMMA on the large ferroelectric crystal phase of P(VDF−HFP) and the barrier effect of the highly insulating two-dimensional (2D) mBNNS, which effectively reduces the relaxation and leakage losses. Our research results show that by using a low-loss matrix and trace high-insulation 2D nanosheets, it is possible to achieve dielectric materials with high η and high U e at the same time.