Lightweight and flexible energy storage devices are gaining interest due to their potential integration into wearable electronics. They might work for the long-term powering of sensors, for example, but they need to be operative after the application of different types of mechanical stress. Conductive and semiconducting nanomaterials have been largely investigated as active components for this type of application but need to be coupled to an elastic matrix, such as a polymeric one, in order to be functional in flexible technologies. In this work, we investigate the production of electrospun nanofibers based on a ternary blend of 2D layered WS2, multiwalled carbon nanotubes, and carbon black in poly(ethylene oxide) and characterize their electrochemical behavior in symmetric supercapacitor architectures within bendable pouch cells, in conjunction with a robust analysis of the active materials’ mechanical properties. We find optimized specific capacitance values of up to 9 F g–1 after mechanical adjustment of the device and excellent capacitance retention after multiple bending cycles, revealing the potential of similar scaffolds for use in wearable energy storage devices to activate low-power electronics.