Various redox-active organic molecules can serve as ideal electrode materials to realize sustainable energy storage systems.Yet,to be more appropriate for practical use,considerable architectural engineering of an ultrathick,high-loaded organic electrode with reliable electrochemical performance is of crucial importance.Here,by utilizing the synergetic effect of the non-covalent functionalization of highly conductive non-oxidized graphene flakes (NOGFs) and introduction of mechanically robust cellulose nanofiber (CNF)-intermingled structure,a very thick (≈ 1 mm),freestanding organic nanohybrid electrode which ensures the superiority in cycle stability and areal capacity is reported.The well-developed ion/electron pathways throughout the entire thickness and the enhanced kinetics of electrochemical reactions in the ultrathick 5,10-dihydro-5,10-dimethylphenazine/NOGF/CNF (DMPZ-NC)cathodes lead to the high areal energy of 9.4 mWh·cm-2 (=864 Wh·kg-1 at 158 W·kg-1).This novel ultrathick electrode architecture provides a general platform for the development of the high-performance organic battery electrodes.