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Nanocomposite Co-LiF and Co-Li3N thin films were successfully fabricated by pulsed laser deposition (PLD). They were investigated as anode materials of lithium ion batteries. Both of Co-LiF and Co-Li3N thin films showed large reversible capacities. The electrochemical products were characterized by high resolution transmission electron microscopy (HRTEM) and selected area electron diffraction (SAED) measurements. Co-LiF and Co-Li3N thin films exhibited different electrochemical reaction mechanism in discharge and charge processes. The results both provide direct evidences that reversible decomposition and formation of LiF and Li3N could be driven by nanosized transition Co metal.