Na-ion hybrid capacitors consisting of battery-type anodes and capacitorstyle cathodes are attracting increasing attention on account of the abundance of sodium-based resources as well as the potential to bridge the gap between batteries (high energy) and supercapacitors (high power). Herein, hierarchically structured carbon materials inspired by multiscale building units of cellulose from nature are assembled with cellulose-based gel electrolytes into Na-ion capacitors. Nonporous hard carbon anodes are obtained through the direct thermal pyrolysis of cellulose nanocrystals. Nitrogendoped carbon cathodes with a coral-like hierarchically porous architecture are prepared via hydrothermal carbonization and activation of cellulose microfibrils. The reversible charge capacity of the anode is 256.9 mAh g −1 when operating at 0.1 A g −1 from 0 to 1.5 V versus Na + /Na, and the discharge capacitance of cathodes tested within 1.5 to 4.2 V versus Na + /Na is 212.4 F g −1 at 0.1 A g −1 . Utilizing Na + and ClO 4 − as charge carriers, the energy density of the full Na-ion capacitor with two asymmetric carbon electrodes can reach 181 Wh kg −1 at 250 W kg −1 , which is one of the highest energy devices reported until now. Combined with macrocellulose-based gel electrolytes, all-cellulose-based quasi-solid-state devices are demonstrated possessing additional advantages in terms of overall sustainability.reserves and their localized geographical availability. [1][2][3] In order to fulfill the complex electrochemical demands of future applications, the development of Na-based energy storage devices with both high energy and power density is of vital importance and necessity; therefore, Na-ion capacitors (NICs) combining a capacitorstyle cathode with a battery-style anode are attractive to balance the gap between batteries and supercapacitors. [4][5][6] To develop cost-competitive NICs, finding low-cost but highly performant materials based on available resources for both electrodes and electrolytes is crucial, particularly when the entire technological scale from synthesis and manufacturing to application and recycling is considered. Recently, significant research efforts have been made to develop novel materials (MoS 2 /MoSe 2 , metal oxide, carbon, etc.) as electrodes for NICs. [7][8][9][10] Among them, sustainable carbon materials inspired from nature, one significant division of the fourth-generation (4G) clean energy technologies, have become one of the up-and-coming candidates for NICs because of their countless advantages including high electrical conductivity, tunable structures, low cost, and stable physicochemical properties. [11][12][13][14] Battery-behaving anodes such as hard carbons have shown promising sodium storage performance and a low volume expansion compared
Sodium-Ion CapacitorsThe ORCID identification number(s) for the author(s) of this article can be found under https://doi.