The extensive usage of portable electronic products and the acceleration of their replacement have led to the discarding of a growing amount of LiCoO2 batteries. It is necessary to recycle the batteries from the both viewpoints of environment and economic benefits. Current recycling approaches for LiCoO2 are dominantly based on hydrometallurgy and pyrometallurgy, which usually require multiple complicated steps and involve the use of high temperature or harmful chemicals, like acids and alkalis. There remains an urgent need for a green and simple process. In this paper, suspension electrolysis technology is proposed to recycle spent batteries, in order to achieve the leaching, purification and regeneration of LiCoO2 in one step. The most advantageous of the present technology are that reacting in one reactor at atmospheric condition and no use of highly corrosive and harmful reagents. The reaction of LiCoO2 leaching in the anode region and simultaneously re-synthesizing in the cathode region in ammonia electrochemical system is established for the first time. This work provides a promising method for recovering LiCoO2 efficiently and environmentally friendly, promoting the sustainable utilization of the resources.