To address the large-scale application demands of high energy density, high power density, and long cycle lifetime, 700-F hybrid capacitor pouch cells have been prepared, comprising ∼240-μm-thick activated carbon cathodes, and ∼60-μm-thick Li4Ti5O12 anodes. Microspherical Li4Ti5O12 (M-LTO) synthesized by spray-drying features 200–400 nm primary particles and interconnected nanopore structures. M-LTO half-cells exhibits high specific capacities (175 mAhh g−1), good rate capabilities (148 mAhh g−1 at 20 C), and ultra-long cycling stabilities (90% specific capacity retention after 10,000 cycles). In addition, the obtained hybrid capacitors comprising activated carbon (AC) and M-LTO shows excellent cell performances, achieving a maximum energy density of 51.65 Wh kg−1, a maximum power density of 2466 W kg−1, and ∼92% capacitance retention after 10,000 cycles, thus meeting the demands for large-scale applications such as trolleybuses.