The research on biodegradable and flexible dielectric materials has been increased widely because of increasing requirements about energy and environmental issues. Polymeric composites with high dielectric constant have, thus, been demanded increasingly compared to ceramic based composites for energy storage devices. The objective of this thesis is to fabricate a biodegradable electrode materials based on pristine and oxidized cellulose nanofibrils (CNF) with different graphene based fillers for enhanced dielectric storage as well as electrochemical charge storage applications. The presented dry method of UV induced reduction of graphene oxide (GO) in cellulose matrices are promising alternatives to solvent based treatments avoiding the deterioration of material properties and the use of organic solvents. This method could be extended to alternative polymer composite materials. In contrast to previous reports, the dielectric properties mainly focussed on the higher frequency regions to provide real, intrinsic material properties and obtained significant enhancement than reported studies. This approach gives a new insight to the exact performance of materials on dielectric charge storage applications. The current study gives more insight for the development of flexible, lightweight and biodegradable electrode materials for energy storage device applications.