CrN thin films have been successfully fabricated by radio frequency sputtering and were investigated for their electrochemistry with lithium for the first time. CrN thin films presented a large reversible discharge capacity around 1200 mAh g(-1). By using ex situ X-ray diffraction, transmission electron microscopy, and selected area electron diffraction measurements, the reversibility of the crystalline structure and electrochemical reaction of CrN with lithium were revealed. The high reversible capacity and good stable cycle of CrN thin film electrode made it one of promising storage energy materials for future rechargeable lithium batteries.