Abstract As a cathode material of aqueous rechargeable zinc‐ion batteries (ARZIBs), molybdenum disulfide (MoS 2 ) still suffers sluggish intercalation kinetics, poor electronic conductivity and insufficient active surface. Here, a hierarchical hybrid composing of ultrathin MoS 2 nanosheets with expanded interlayer spacing that grow directly on the surface of carbon nanotubes (MoS 2 @CNTs) is firstly proposed as the cathode material of ARZIBs. Its zinc storage performance and corresponding enhanced mechanism are investigated via electrochemical characterizations and density functional theory calculations. The results reveal that the enlarged spacing of MoS 2 interlayer decreases the energy barrier of Zn 2+ intercalation and the CNTs backbone improves the electron transfer. What's more, the hierarchical structure provides a great number of active sites for electrochemical reactions. As a result, the hierarchical MoS 2 @CNTs hybrid delivers a high reversible capacity with good cycling stability and rate capability.