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Designing energy storage devices from thick carbon electrodes with high areal/volumetric energy density via a simple and green way is very attractive but still challenging. Cellulose, as an excellent precursor for thick carbon electrodes with abundant sources and low cost, is usually activated by a chemical activator and pyrolysis route to achieve high electrochemical performance. However, there are still some problems to be addressed, such as the harsh activation conditions, easy collapse of porous structures, and the high cost. Herein, a 3D self‐supporting thick carbon electrode derived from wood‐based cellulose is proposed for high areal and volumetric energy density of supercapacitor from a mild, simple, and green enzymolysis treatment. Benefiting from the high specific surface area (1418 m2 g−1) and abundant active sites on the surface of wood‐derived hierarchically porous structures and enzymolysis‐induced micropores and mesopores, the assembled symmetry supercapacitor from the thick carbon electrode can realize the high areal/volumetric energy density of 0.21 mWh cm−2/0.99 mWh cm−3 with excellent stability of 86.58% after 15 000 long‐term cycles at 20 mA cm−2. Significantly, the simple and universal strategy to design material with high specific surface area, provides a new research idea for realizing multi‐functional application. [ABSTRACT FROM AUTHOR]

[Display omitted] • The effect of electrode thickness on the supercapacitance performance is studied. • Bass wood with hierarchical pores is easy processed to thick electrode. • The thick electrodes have high specific/areal/volumetric energy/power densities. • The SSC shows excellent cycling performance of 81% (20 mA cm−2, 15 000 cycles). The practical application of energy storage device requires high areal/volumetric energy density. One of the strategies is to design bulk electrode with hierarchical porous structure for the application of supercapacitor. Significantly, the energy storage electrochemical performance of the bulk electrode is highly influenced by the pore structure regulation and electrolyte infiltration. Therefore, it is necessary to design thick electrodes with proper pore structures and investigate the effect of thickness on the supercapacitance performance. In this work, bass wood is selected as the carbon source of electrode because of its hierarchical porous structure and easy processing into different thicknesses. The wood-derived carbon thick electrode with a thickness of 1.532 mm (CWT1.532) presents the best supercapacitance performance. Such electrode possesses a high active material loading of 54.75 mg cm−2. The symmetrical supercapacitor from CWT1.532 electrode displays remarkable specific capacitance of 65 F g−1 and areal/volumetric capacitance of 0.846 F cm−2 and 2.67 F cm−3 at 1.0 mA cm−2, respectively. It also exhibits mass/areal/volumetric power densities of 38.47 W kg−1, 500 mW cm2 and 1580 mW cm−3 as well as the corresponding energy densities of 9.04 Wh kg−1, 117.5 mWh cm−2 and 0.374 mWh cm−3, respectively. Moreover, the symmetrical supercapacitor shows an attractive cycling stability with a supercapacitance retention of 81.48% at 20 mA cm−2 even after 15 000 long-term cycles. This work provides an essential understanding about the effect of different thicknesses on the thick electrode-assembled supercapacitance and inspires future practical application in other energy storage areas. [ABSTRACT FROM AUTHOR]