Iron carbide-functionalized porous carbon nanocomposites are considered as potential anode materials for lithiumion batteries (LIBs) for their good electrocatalytic performance, stable chemical properties, and reasonable cost-effectiveness. In this work, a unified Fe 3 C-functionalized 3D nitrogen-doped porous graphene nanocomposite (Fe 3 C/NPG) was synthesized using a simple strategy that involved the coordination of silk fibroin with Fe ions. This material exhibited a distinct 3D porous structure, high doping levels of nitrogen atoms (approximately 10%), and well-dispersed Fe 3 C nanoparticles with strong interfacial bonding. The Fe 3 C/NPG composite demonstrated excellent reversible capacity and rate performance as a LIB anode material at a heating temperature of 800 °C and a Fe ion concentration of 50 mM. It exhibited a rate capacity of 729.5 mA h/g at 0.1 A/g and a discharge capacity of 205.5 mA h/g after 200 cycles at a high current density of 4.0 A/g. Overall, Fe 3 C/NPG shows great potential as an anode material for LIBs due to its outstanding cycling stability and impressive rate capabilities.