Polymers have been considered as promising materials for dielectric energy storage because of their high breakdown strength, favorable flexibility and processability. The achievable energy density of polymers is however limited by their intrinsic low dielectric constant. Until today, most of them are either melt-extruded at high temperatures or solutionprocessed in harmful organic solvents. Making high-energy polymeric dielectrics via environmentally friendly manners has been a long standing challenge. Herein, a water-based technique is employed to prepare all-polymeric dielectrics consisting of poly(vinylidene fluoride) (PVDF) latex nanoparticles dispersed within a polyvinyl alcohol (PVA) matrix. These waterborne nanocomposites, processed at low temperature, demonstrate great promise in resolving the paradox between dielectric constant and breakdown strength. A high energy density of 8.1 J/cm 3 is thus achieved at ~515 MV/m, which is 300% greater than that of each polymer component. Moreover, with an appropriate load resistance, the nanocomposite can release the stored energy at a rate of microseconds, giving rise to a power density of 1.13 MW/cm 3 that is nearly 400% higher than that of benchmark biaxial oriented polypropylene dielectric films.