Abstract

Abstract Layered materials have great potential as cathodes for aqueous zinc‐ion batteries (AZIBs) because of their facile 2D Zn 2+ transport channels; however, either low capacity or poor cycling stability limits their practical applications. Herein, two classical layered materials are innovatively combined by intercalating graphene into MoS 2 gallery, which results in significantly enlarged MoS 2 interlayers (from 0.62 to 1.16 nm) and enhanced hydrophilicity. The sandwich‐structured MoS 2 /graphene nanosheets self‐assemble into a flower‐like architecture that facilitates Zn‐ion diffusion, promotes electrolyte infiltration, and ensures high structural stability. Therefore, this novel MoS 2 /graphene nanocomposite exhibits exceptional high‐rate capability (285.4 mA h g −1 at 0.05 A g −1 with 141.6 mA h g −1 at 5 A g −1 ) and long‐term cycling stability (88.2% capacity retention after 1800 cycles). The superior Zn 2+ migration kinetics and desirable pseudocapacitive behaviors are confirmed by electrochemical measurements and density functional theory computations. The energy storage mechanism regarding the highly reversible phase transition between 2H‐ and 1T‐MoS 2 upon Zn‐ion insertion/extraction is elucidated through ex situ investigations. As a proof of concept, a flexible quasi‐solid‐state zinc‐ion battery employing the MoS 2 /graphene cathode demonstrates great stability under different bending conditions. This study paves a new direction for the design and on‐going development of 2D materials as high‐performance cathodes for AZIBs.