Flexible electronic devices are portable, wearable, bendable, and foldable and are becoming critical for connecting a new round of application upgrades and technological revolutions. [1] In this context, wearable electronic devices, such as electronic sensors, flexible displays, artificial electronic skin, backup power supplies, and health monitors, have attracted considerable attention, with rapid developments being reported. [2][3][4][5][6] The design and manufacture of lightweight electrochemical energy storage devices with flexibility, high energy density, and power density have become crucial to meet the power requirements of these electronic devices. [7,8] Traditional rigid energy storage devices represented by lead-acid batteries, [9] lithiumsulfur batteries, [10,11] and lithium-ion batteries [12] are likely to suffer equipment performance degradation or even damage when bent or folded, limiting their use in flexible electronic equipment. Therefore, there is a need to develop new energy storage systems compatible with flexible electronic devices. In this regard, flexible hybrid devices with excellent mechanical properties, higher power density, longer cycle life, rapid charge storage capacity, and excellent safety are needed to provide power sources for flexible and lightweight electronic equipment. [13][14][15][16][17] As pivotal components of flexible hybrid devices, electrode materials determine the properties of the energy storage device, such as energy density, power density, cycle life, and flexibility. [18] Therefore, the development of advanced electrode materials is the key to the fabrication of high-performance flexible devices for energy storage.Transition metal sulfides have attracted considerable attention owing to their excellent chemical and physical properties. For example, CoS, MnS, Ni 3 S 2 , SnS, and MoS 2 are used widely as anode materials for hybrid devices. [19][20][21][22][23] Among the various transition metal sulfides available, CuS is made from high earthabundant elements, has low cost, and is environmentally friendly; thus, it has been used widely in various fields. [24] As an important p-type semiconductor material, CuS is expected to become a candidate electrode material for energy storing owing to its good safety and large theoretical specific capacity. [25][26][27][28] However, the insufficient electronic conductivity of CuS causes the volume expansion of the material during the charging and discharging process, resulting in serious mechanical deformation and the rapid capacity fading of the electrode material, which greatly limits its application as an active electrode material. [29] To overcome these obstacles, considerable research has focused on the construction of new CuS composites, such as