Ultrathick MoS2 Films with Exceptionally High Volumetric Capacitance

Abstract Manufacturing electrode films at an industrial‐level submillimeter thickness (≈100 µm) with superior volumetric performance is of practical significance for the commercialization of miniaturized supercapacitor systems. This work proposes a commercially scalable solvated‐ion‐intercalated hydrothermal strategy to demonstrate a record‐high volumetric capacitance (511.29 F cm −3 ) for supercapacitors based on an industrial‐level submillimeter MoS 2 film electrode (94.2 µm). The intercalated solvated Li + ions increase the amount of negative surface charge and reduce the formation energy of 1T MoS 2 , leading to a high metallic phase content of 82.7% with enhanced electrical conductivity. Together with the expanded interlayer distance (≈1.23 nm), this allows rapid electron transfer and ion transport in the excessively stacked ultrathick MoS 2 film to be simultaneously realized. Thus, the as‐fabricated MoS 2 ||graphene/carbon nanotube asymmetric supercapacitor presents both high energy and power densities, outperforms those of commercial devices, including supercapacitors with submillimeter‐thick electrodes and even micrometer‐thick electrodes.