▎ 摘　　要

The push toward high-performance supercapacitors calls for the development of efficient pseudocapacitive negative electrode materials that can better match the high capacitance of the typical positive electrodes. Herein, a facile and one-pot hydrothermal approach for the in situ growth of the nickel-zinc-iron layered double hydroxide (LDH) onto the graphene aerogel (GA) substrate is introduced. Proper selection of the metal precursors with prominent pseudocapacitive behavior over a wide potential range coupled with the excellent double-layer capacitive and charge transport properties of the GA network results in an LDH-GA nanocomposite that displays outstanding supercapacitive performances as both negative (387 F g(-1), 101 mA h g(-1), at 1.0 A g(-1)) and positive (1235 F g(-1), 103 mA h g(-1)) electrodes. An aqueous LDH-GA//LDH-GA device with a wide voltage window (1.55 V) that demonstrates a significantly enhanced specific capacitance (304 F g(-1) at 1.0 A g(-1)), outstanding specific energy (95 W h kg(-1)), appreciable specific power (81 kW kg(-1)), along with 88% retention of the initial capacitance after 10 000 cycles, is also fabricated. The superior supercapacitive performance of the Ni-Zn-Fe LDH-GA nanocomposite over both negative and positive voltage ranges opens a promising pathway toward manufacturing high-energy supercapacitors for state-of-the-art applications.