The paper presents a novel approach to enhance the performance of aqueous zinc-ion batteries (AZIBs) by integrating VS₂ nanosheets into MXene interlayers to form a stable 2D heterogeneous layered structure. This structure improves the stability, conductivity, and ion transport of the electrode materials, leading to high specific capacity and long-term cycling stability. The VS₂/Ti₃C₂Tx composite film, when used as both the cathode and anode in AZIBs, demonstrates excellent electrochemical properties, including a high specific capacity of 285 mAh g⁻¹ at 0.2 A g⁻¹ and a capacity retention of 97% after 5000 cycles. Additionally, a flexible Zn-metal-free in-plane VS₂/Ti₃C₂Tx//MnO₂/CNT AZIB shows high operation voltage (2.0 V) and outstanding long-term cycling stability, making it a promising candidate for wearable device applications. The study highlights the potential of this composite material in advancing the development of high-performance AZIBs.The paper presents a novel approach to enhance the performance of aqueous zinc-ion batteries (AZIBs) by integrating VS₂ nanosheets into MXene interlayers to form a stable 2D heterogeneous layered structure. This structure improves the stability, conductivity, and ion transport of the electrode materials, leading to high specific capacity and long-term cycling stability. The VS₂/Ti₃C₂Tx composite film, when used as both the cathode and anode in AZIBs, demonstrates excellent electrochemical properties, including a high specific capacity of 285 mAh g⁻¹ at 0.2 A g⁻¹ and a capacity retention of 97% after 5000 cycles. Additionally, a flexible Zn-metal-free in-plane VS₂/Ti₃C₂Tx//MnO₂/CNT AZIB shows high operation voltage (2.0 V) and outstanding long-term cycling stability, making it a promising candidate for wearable device applications. The study highlights the potential of this composite material in advancing the development of high-performance AZIBs.