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Chitosan-based carbon materials have attracted great attention in electrochemical energy storage. Introducing iron metal or iron compounds into carbon materials favors to boost their electrochemical performance. Herein, chitosan-based graphitic carbon@Fe3C composites (CSGC@Fe3C) have been prepared as anode materials for lithium ion battery by a simple pyrolysis method. By manipulating the temperature higher than 700 °C, pure Fe3C encapsulated in chitosan-based graphitic carbon with different mass ratio from 30 to 53.8 wt% can be achieved. The resulting CSGC@Fe3C composites retain porous carbon sheet structure embedded with a large amount of Fe3C nanoparticles in size from 20 to 300 nm. The electrochemical measurements demonstrate CSGC@Fe3C with 53.8 wt% Fe3C as anode material for lithium ion battery can provide a highest reversible capacity of 423 mAh g−1 at 0.1 A g−1 over 100 charge/discharge cycles and stable cycling capacity of 195 mAh g−1 at a high current density of 2 A g−1 during 200 cycles. The catalysis of Fe3C on the reversible formation and decomposition of solid electrolyte interphase (SEI) has been corroborated and results in the improvement of surface capacitive contribution. This work provides a basic insight into metal carbides constructing biomass-based carbon anode materials to realize high-performance electrochemical energy storage device. [ABSTRACT FROM AUTHOR]