in LIBs are mostly organic and harmful, which inevitably enhance the difficulty and the cost of battery fabrication and also bring about some environmental impact. [3] As an alternative, rechargeable aqueous zinc-ion batteries (ZIBs) have shown great promise because of low toxicity, low cost, and the abundant distribution of zinc resources. [4] More importantly, zinc possesses a low redox potential (−0.762 V vs. standard hydrogen electrode) and a high theoretical capacity (819 mAh g −1 , 5851 mAh mL −1 ). [4d] Furthermore, zinc is stable in water, which can reduce the production cost and improve the safety. [5] Despite these advantages, it is a large challenge to develop a high-performance cathode material for aqueous ZIBs that provides high and stable capacities and keeps the structure integrity in Zn 2+ uptake, which is mainly due to heavy mass and high polarization of divalent Zn 2+ . Among various reported cathode materials (such as α, β, γ, and δ-MnO 2 , [4c,6] Prussian blue analogs, [7] Na 3 V 2 (PO 4 ) 3 , [8] and vanadium-based materials [9] ), vanadium pentoxide (V 2 O 5 ) is of particular interest owing to its high Zn 2+ ion storage capacity (≈590 mAh g −1 according to the two-electron redox center of vanadium) in its layered structure consisting of VO 5 units. [10] Unfortunately, V 2 O 5 cathodes exhibit rapid capacity decline during (de)intercalation of Zn 2+ due to the low ion diffusion coefficient, poor conductivity, elements dissolution, and selfaggregation. [11] To overcome this drawback, it has been reported that intercalation of H 2 O molecules into the interlayers of V 2 O 5 could effectively enlarge and maintain the layered configuration of V 2 O 5 -based materials, which offered high Zn 2+ ion storage capability and stable cycling performance. [5c,12] Also, by inserting other metallic ions such as Ca 2+ , [9a] Zn 2+ , [9e] Na + , [13] or Li + , [14] the formation of metal vanadium oxide bronzes has been demonstrated to enhance Zn 2+ storage performances. The typical structure of these metal vanadates is that the V-O layers expand along the c-axis while the intercalated metal ions and H 2 O molecules stay in the interlayer space. [15] Despite significant progress, further boosting the Zn 2+ storage ability of V 2 O 5 -based cathodes through other strategies is still urgently required, particularly at large rates.As a highly conductive and extremely stable polymer, poly(3,4-ethylenedioxythiophene) (PEDOT) has been reported to not only effectively improve the electronic conductivity of Aqueous zinc-ion batteries (ZIBs) have become research focus because of their cost-effectiveness, high safety, and eco-friendliness. Unfortunately, sluggish Zn 2+ diffusion kinetics and the poor cycling stability in cathode materials impede their large-scale application. Herein, V 2 O 5 @poly(3,4ethylenedioxythiophene) (PEDOT) hybrid nanosheet arrays are uniformly deposited on carbon cloth (CC) as a superior ZIB cathode. The as-fabricated V 2 O 5 @PEDOT/CC electrode displays a maximum capacity of 360 mAh ...