The advancement of new dielectric materials exhibiting greater discharge energy density is crucial for current power systems and electronic devices. In this work, various weight percentages of graphene oxide@zinc oxide (GO@ZO) nanofillers were incorporated inside a polymer blend of poly(vinylidene fluoride-hexafluoropropylene)/polyetherimide (P(VDF-HFP)/PEI; shortened as BP) and used as a high dielectric top layer. In contrast, linear-type PEI (L) was used as a bottom insulation layer to achieve a high breakdown strength (Eb) in bilayer nanocomposites. As a result, the 2BP-L composite demonstrated a high discharged energy density of 12.63 J/cm3 at an electric field of 527 MV/m with only 2 wt% GO@ZO nanofillers addition in the top layer. Such a high discharge energy density with minimal nanofiller loading is attributed to the utilization of novel surface-decorated GO@ZO nanofillers and new bilayer-heterostructured linear/ferroelectric-linear polymer. In comparison to its counterparts (i.e., PEI, P(VDF-HFP) and 0BP-L), the 2BP-L nanocomposite showed ∼426.3 %, 92.5 %, and 9.8 % enhancement in discharge energy density, respectively. The discharge rate and stability analysis revealed a significantly higher power density of 0.55 MW/cm3, indicating its high potential to be used as a pulsed power system. Finite element simulation revealed that the effective internal electric field distribution and higher dielectric displacement in 2BP-L resulted in such enhancement over its counterparts. This study presents a new model to maximize the energy storage capability of flexible energy storage devices and advances knowledge of the polarization mechanisms and breakdown of bilayer nanocomposite dielectric materials.