prevent them from migrating in the electrolyte solutions between the negative and positive electrodes, which generate shuttle effect to lead to energy loss. [3] In addition, the carbon substrate can also help active organic molecules to release energy storage performances due to the high electrical conductivity and good electrochemical catalysis. In the Li-ion batteries, lots of organic molecules have been selected to prepare OMEs, such as organodisulfides, conducting polymers, conjugated carbonyl compounds, and nitroxyl radical polymers. [4,5] Especially, the carbonyl organic compounds as potential electrode candidates have been widely studied because of their large theoretical capacity, structural diversity, and inexpensive. For instance, calix[4]quinone (422 mAh g −1 vs Li/Li + ), [6] 1,4-benzoquinone (157 mAh g −1 vs Li/Li + ), [7] 1,4-bis(pbenzoquinonyl)benzene (306 mAh g −1 vs Li/Li + ), [8] and so on have been proven to exhibit excellent performance in specific capacity. Actually, the OMEs can not only store charges through redox reactions of groups on the molecular skeletons but also contribute electrical double layer capacitance to the whole electrode due to the surface electrochemical properties of conductive carbon substrates. Therefore, OMEs has become increasingly popular in the electrode applications for supercapacitors (SCs). In recent years, the organic molecules with benzoquinone structure, especially quinones (phenols) and their derivatives, have represented a tremendous potential to achieve super-capacitive performances in terms of larger capacitance, long-cycle life, and high-rate capability. [9] For example, Gogotsi et al. found that 2,5-dimethoxy-1,4-benzoquinone (DMQ) immobilized reduced graphene oxide (rGO) to form DMQ@rGO composite under the hydrothermal conditions. It is noted that the DMQ@rGO acquires excellent specific capacitance (600 F g −1 ) with outstanding capacitance retention (99%). [10] Wang et al. used the sodium anthraquinone-2-sulfonate (AQS) to functionalize the rGO sheets and prepared an AQS@rGO electrode with larger specific capacitance (567.1 F g −1 ) and long cycling-life (89.1% over 10 000 cycles). [11] Available commercialized quinones (phenols) molecules are less in categories and insufficiently variable in the A new redox-active organic molecule, naphthalene diimide derivative (NDI), is synthesized through the condensation reaction for electrochemical energy storage, in which 1,4,5,8-naphthalenetetracarboxylic dianhydride and 4-aminophenol are used as skeleton and substituent, respectively. The NDI is acted as a guest molecule to non-covalently modify reduced graphene oxide (rGO) and to form an organic molecular electrode (OMEs). The resultant electrode exhibits outstanding performance under the three-electrode configuration, including specific capacitance (354 F g −1 at 5 mV s −1 ) and cycling performance (87.2% after 8000 cycles). Furthermore, the electrochemical behaviors of the OMEs are mainly controlled by surface reactions and pseudocapacitance contribution is...