There is an urgent need to develop gel electrolytes with excellent mechanical properties, deformability, and fatigue resistance to meet the flexibility requirements of novel supercapacitors. In this paper, polyacrylonitrile nanosphere-nanocomposite (PANNS-NC) hydrogels were synthesized by incorporating polyacrylonitrile nanospheres as reinforcing agents and employing N, N'-Methylenebis(acrylamide) (MBA) and N, N'-hexamethylenebisacrylamide (SMBA) as crosslinkers to achieve both physical and chemical crosslinking. The resulting PANNS-NC hydrogels demonstrated exceptional mechanical properties, including an ultrahigh elongation of 2380% and a remarkable tensile strength of 229.6 kPa. The gel electrolyte prepared from the PANNS-NC exhibited an ultrahigh ionic conductivity of 0.34 S·cm−1 and remarkable fatigue resistance, indicated by the absence of structural damage even after 1000 compression and tension cycles. Furthermore, the assembled supercapacitor demonstrated exceptional cycling stability, with a capacitance retention rate of 93% after 10,000 compression cycles with 50% strain. It maintained a 100% capacitance retention rate after 10,000 cycles with 90° bending. PANNS-NC holds great promise for use as a gel electrolyte material in supercapacitor development. Additionally, its suitability extends beyond supercapacitors, as it represents a novel material option for various other flexible devices.