Fluoropolymer/inorganic nanofiller composites are considered to be ideal polymer dielectrics for energy storage applications because of their high dielectric constant and high breakdown strength. However, these advantages are a trade-off with the unavoidable aggregation of the inorganic nanofillers, which result in a reduced discharge of the energy storage density. To address this problem, we developed polyvinylidene fluoride (PVDF) graft copolymer/cellulose-derivative composites to achieve high-dielectric and energy-storage density properties. An enhanced dielectric constant and improved energy density were achieved with this structure. The optimal composites exhibited a high discharge energy density of 8.40 J/cm3at 300 MV/m. This work provides new insight into the development of all-organic composites with bio-based nanofillers.