Energy storage technologies such as lithium-ion batteries (LIBs) and electrochemical capacitors (ECs) are currently the focus of intense research for applications that include electronic devices and electric vehicles. [1][2][3] Owing to the different energy storage mechanisms, batteries are able to deliver high energy density, while ECs have comparatively lower energy density but higher power density and longer cycling stability. [4][5][6] The expected technological advancements and increase in global energy consumption over the next decades will require energy storage devices with higher power densities, large capacities, and longer lifespans, compared to those currently available.Nonaqueous hybrid supercapacitors (HSCs), which generally consist of a battery-type anode (e.g., LIB) and an EC cathode in order to combine the advantages of both system storage mechanisms, are promising energy storage systems to meet future energy demands. [7][8][9] HSCs cathode materials are typically high surface area carbons, with the charge stored at the interface between the electrode and liquid electrolyte, and show high power density, high rate capability, and cycling stability. [10,11] At the battery-type anode, charges are usually stored through a Li + intercalation mechanism. [12] Therefore, the rate performance of HSCs is limited by the slow kinetics of lithium diffusion in the solid, as the surface adsorption-desorption processes at the cathode are considerably faster than the Faradaic reactions that take place at the anode. [13,14] Several materials, including Nb 2 O 5 , [15][16][17] Li 4 Ti 5 O 12 , [18] TiO 2 , [19] V 2 O 5 , [20] VN, [21] and MnO, [22] are being investigated as anodes to fabricate HSCs. In particular, Nb 2 O 5 shows promise due to its high theoretical specific capacity (≈200 mAh g −1 ), fast Li ions' diffusion, and good cycling stability. [23] Despite the charge storage deriving from the insertion of Li ions into the structure, the electrochemical behavior of Nb 2 O 5 is similar to that of a pseudocapacitive material. This mechanism has been named intercalation pseudocapacitance, and it is characterized by fast Faradaic processes occurring during ion insertion-deinsertion into the host material. [8] It has been demonstrated that the performance of Nb 2 O 5 strongly Efficient synthetic methods to produce high-performance electrode-active materials are crucial for developing energy storage devices for large-scale applications, such as hybrid supercapacitors (HSCs). Here, an effective approach to obtain controllable carbon-encapsulated T-Nb 2 O 5 nanocrystals (NCs) is presented, based on the solvothermal treatment of NbCl 5 in acetophenone. Two separate condensation reactions of acetophenone generate an intimate and homogeneous mixture of Nb 2 O 5 particles and 1,3,5-triphenylbenzene (TPB), which acts as a unique carbon precursor. The electrochemical performance of the resulting composites as anode electrode materials can be tuned by varying the Nb 2 O 5 /TPB ratio. Remarkable performances are achieved fo...