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Supercapacitors (SCs) are becoming new candidates in the field of sustainable energy supply. Nevertheless, the unsatisfactory energy density due to the narrow voltage window of the supercapacitor is the main barrier to its practical application. Developing appropriate electrode materials to improve the electrochemical performance of SCs and broaden the operating voltage of supercapacitors are imperative. Herein, compatible interfacial engineering wood-derived nanostructured electrodes for aqueous asymmetric supercapacitors (AASCs) are demonstrated. The 3D carbonized wood matrix serves as a high specific surface area current collector and a porous host for the high capacitive active substance, which is composed of manganese dioxide (MnO2) nanowires and polyaniline (PANI) nanoparticles grown uniformly on the porous wall of aligned microchannels (CW@MnO2 and CW@PANI). The resulting electrochemical exchange reactive sites enable the positive electrode to deliver a high areal capacitance of 729 mF cm−2 at 1 mA cm−2 (369 F g−1 at 0.5 A g−1). The negative electrode delivers a high areal capacitance of 1721 mF cm−2 at 1 mA cm−2 (848 F g−1 at 0.5 A g−1). The areal capacitance of two electrodes is superior to most reported supercapacitor electrodes. Additionally, the assembled CW@MnO2//CW@PANI AASC achieves a desirable energy density (170.84 μWh cm−2 at a power density of 0.5 mW cm−2) because a considerable work function difference between electrodes achieved a 2 V wide voltage window. The results of this study provide a critical benchmark and optimistic incentives to adopt natural hierarchical structures to enhance the performance of new-generation energy-related systems.