Abstract: Fe₃O₄ is an attractive alloy-type anode material because of its high known capacity (924mAh/g). However, Li⁺ insertion into and extraction from Fe₃O₄are accompanied by a huge volume change,up to 90%, which induces a strong strain on Fe₃O₄ and causes pulverization and rapid capacity fading due to theloss of the electrical contact between part of Fe₃O₄ and current collector.We report an advanced Lithium-ion battery based on a free standing carbon nanofiber paper(CNP) ink and Fe₃O₄ anode that overcome the pulverization problem. The Fe₃O₄ nanoparticles were electrochemically grown on self-supported CNP. It could be used as a kind of metallic-free current collector anode for Lithium-ion battery, which would significantly reduce the mass of the whole anode by 66 %. The new flexible Fe₃O₄/CNP composite anode achieves a higher initial reversible capacity of 1120 mAh/g and exhibits more stable performance compared with Fe₃O₄ anode coated on Cu foil by traditional electrode-fabrication technique. This is due to that the flexible 3D porous structured Fe₃O₄/CNP composite is light weight and can accommodate the volume change of Fe₃O₄ during the lithiation/delithiation process, and promotes the diffusion and transfer of lithium ionand electron, respectively. Compared with the pure Fe₃O₄nanoparticles, the Fe₃O₄/CNP exhibited a better cycling stability, because the carbon nanofiber with high mechanical strength and elasticity can work as a buffer to prevent the volume expansion and contraction of Fe₃O₄ nanoparticles during the Li⁺ insertion/extraction process. Meanwhile, compared with single CNP, the Fe₃O₄/CNP showed a higher capacity because of the hybridizing with higher capacity Fe₃O₄ nanoparticles. Moreover, this Fe₃O₄/CNP composite anode displays excellent rate capability, which maintains a discharge specific capacity of 210 mAh/g when the applied current rate is 10 C and still delivers 1150 mAh/g after returning to 0.2C. The excellent electrochemical performance of the Fe₃O₄/CNP as an anode material in Lithium-ion battery was obtained. Our work provides a new way to develop novel electrode structure for light-weighted and flexible Lithium-ion battery.