Transition metal phosphides are promising anode materials for lithium ion batteries because of their abundant natural resources and high theoretical capacities. In this study, the electrochemical properties of LiFeP as an anode material for lithium ion battery were investigated for the first time. LiFeP powders were successfully synthesized by a conventional two-step solid-state reaction method. The results of X-ray powder diffraction and selected area electron diffraction revealed that the layered plate-like LiFeP was stacked by the (001) crystal plane. As an electrode material, LiFeP delivered a superior reversible capacity of 507 mA h g−1 at a high current density of 300 mA g−1 after 300 cycles and excellent rate performance. After cycling, the layered structure can be well maintained, which would be greatly beneficial to the electrochemical performance of LiFeP. The reason for the increase in capacity was also investigated and can be attributed to the high number of conversion reactions of LiFeP and the generation of elemental P during cycling.