Flexible vanadium and nitrogen co-modified amorphous carbon nonwoven films are successfully synthesized and applied as free-standing film anodes for lithium-ion batteries (LIBs). The developed films exhibit outstanding capacity with an initial Coulombic efficiency of 63.3%. Furthermore, favorable rate capability and good cycling stability are achieved. Cycling at a current density of 0.1 A g⁻¹, the specific capacity of the nitrogen doped V-O-C nanofiber film reaches as high as 1380 mA h g⁻¹, showing considerable promise for use as an electrode for flexible lithium-ion batteries.