The commonly used metal thin film or resin-based flexible composites cannot meet the requirement of cryogenic flexible conductive functional devices, which may be used in space exploration, biomedicine, and other science and technology fields facing a very low temperature environment, because of their poor fatigue and anti-bending properties at cryogenic temperature. In this work, a composite based on functionalized cotton fibers is proposed to achieve the application requirement of flexible electrical systems at cryogenic temperature. A conductive composite film with optimized strength and flexibility was obtained by controlling the size distribution of cotton fibers and adjusting the interaction force among the cotton fibers. The obtained composite film could endure over 10,000 times of bending at 77 K (−196 °C), with the resistance changing less than ±5%, indicating its excellent mechanical flexibility and electrical stability at cryogenic temperature. Finally, a demonstration was successfully conducted by applying the composite film as a flexible electrical connection to a robot arm, which worked at 77 K. This work might be a reference significance for the application of flexible conductors from room temperature to cryogenic temperature.