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Summary: The pyrolysis of metal‐organic frameworks (MOFs) to derive porous nanocarbons and metal oxides has attracted scientific attention due to the advantageous properties of the final products (eg, high surface areas). In the present research, MIL‐125 (MIL = Materials of Institute Lavoisier, a Ti‐based MOF) has been subjected to a single‐step pyrolysis treatment in argon atmosphere. The combination of uniformly linked titanium metal cluster and oxygen‐enriched organic linker has acted as a template to yield a titanium dioxide (TiO2)–carbon nanocomposite. The TiO2 nanoparticles infused in carbon skeleton structure (TiO2/C) has been investigated as an electrode material for supercapacitor applications. TiO2/C electrodes have delivered an excellent electrochemical performance, for example, in terms of charging–discharging efficiency. Two equally weighed TiO2/C electrodes have been used to assemble a solid‐state symmetrical supercapacitor (SC) device, containing a gel electrolyte (poly vinyl alcohol in 1 M H2SO4). The above device has delivered a high value of energy density (43.5 Wh/kg) and an excellent power output of 0.865 kW/kg. The symmetrical SC could retain almost 95% of its initial capacitance even after 2000 charging–discharging cycles. The electrochemical performance of the TiO2/C SC was better than most MOF‐based SCs reported previously. Such performance is attributed to the synergistic combination of electrically conducting MOF‐derived carbon and redox active TiO2 nanocrystals with a large specific surface area. [ABSTRACT FROM AUTHOR]