The design of advanced high-energy-density supercapacitors requires the design of unique materials that combine hierarchical nanoporous structures with high surface area to facilitate ion transport and excellent electrolyte permeability. Here, shape-controlled 2D nanoporous carbon sheets (NPSs) with graphitic wall structure through the pyrolysis of metal-organic frameworks (MOFs) are developed. As a proof-of-concept application, the obtained NPSs are used as the electrode material for a supercapacitor. The carbon-sheet-based symmetric cell shows an ultrahigh Brunauer-Emmett-Teller (BET)-area-normalized capacitance of 21.4 µF cm-2 (233 F g-1 ), exceeding other carbon-based supercapacitors. The addition of potassium iodide as redox-active species in a sulfuric acid (supporting electrolyte) leads to the ground-breaking enhancement in the energy density up to 90 Wh kg-1 , which is higher than commercial aqueous rechargeable batteries, maintaining its superior power density. Thus, the new material provides a double profits strategy such as battery-level energy and capacitor-level power density.

Catalan Institute of Nanoscience and Nanotechnology CSIC and the Barcelona Institute of Science and Technology Campus UAB Bellaterra 08193 Barcelona Spain

Chair of Inorganic and Metal Organic Chemistry Department of Chemistry and Catalysis Research Centre Technical University of Munich 85748 Garching Germany

Regional Centre of Advanced Technologies and Materials Faculty of Science Palacky University Olomouc Šlechtitelů 27 783 71 Olomouc Czech Republic

School of Chemical Engineering The University of Adelaide Adelaide South Australia 5005 Australia

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