Abstract: | The development of cost‐effective and flexible electrodes is demanding in the field of energy storage. Herein, flexible FexOy/nitrogen‐doped carbon films (FexOy/NC‐MOG) are prepared by facile electrospinning of Fe‐based metal–organic gels (MOGs) followed by high‐temperature carbonization. This approach allows the even mixing of fragile coordination polymers with polyacrylonitrile into flexible films while reserving the structural characteristics of coordination polymers. After thermal treatment, FexOy/NC‐MOG films possess uniformly distributed FexOy nanoparticles and larger accessible surface areas than traditional FexOy‐NC films without MOG. Taking advantage of the unique structure, FexOy/NC‐MOG exhibits a superior rate performance (449.8 mA h g?1 at 5000 mA g–1) and long cycle life (629.3 mA h g–1 after 500 cycles at 1000 mA g–1) when used as additive‐free anodes in lithium‐ion batteries. |