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Abstract  To fabricate battery‐like supercapacitors with high power and energy densities, big capacitances, as well as long‐term capacitance retention, vertically aligned carbon nanofibers (CNFs) grown on boron doped diamond (BDD) films are employed as the capacitor electrodes. They possess large surface areas, high conductivity, high stability, and importantly are free of binder. The large surface areas result from their porous structures. The containment of graphene layers and copper metal catalysts inside CNFs leads to their high conductivity. Both electrical double layer capacitors (EDLCs) in inert solutions and pseudocapacitors (PCs) using Fe(CN) 6  3−/4−  redox‐active electrolytes are constructed with three‐ and two‐electrode systems. The assembled two‐electrode symmetrical supercapacitor devices exhibit capacitances of 30 and 48 mF cm −2  at 10 mV s −1  for EDLC and PC devices, respectively. They remain constant even after 10 000 charging/discharging cycles. The power densities are 27.3 and 25.3 kW kg −1  for EDLC and PC devices, together with their energy densities of 22.9 and 44.1 W h kg −1 , respectively. The performance of these devices is superior to most of the reported supercapacitors and batteries. Vertically aligned CNF/BDD hybrid films are thus useful to construct high‐performance battery‐like and industry‐orientated supercapacitors for future power devices.

Battery‐like Supercapacitors from Vertically Aligned Carbon Nanofiber Coated Diamond: Design and Demonstrator