In order to solve the problems of complicated operation and high cost existing in traditional preparation technology, the pure phase lithium titanate (LTO) / copper foil (Cu) thin film electrode without adhesive was successfully prepared by microelectronic ink jet printing combined with high temperature annealing. Scanning electron microscope analysis results show that the pure phase LTO with nanoparticle shape can be uniformly deposited on the surface of Cu. The button cell assembled with 10 layers of active material LTO / Cu film electrode and Li negative electrode by inkjet printing has a specific capacity of 91.27 mA·h/g at 3C (1.0 ~ 1.7 V) current density, and after 1000 cycles, the retention rate of discharge specific capacity is 85.4%, which show excellent cycle stability. The above results show that the method of inkjet printing combined with high temperature annealing has a broad application prospect in the preparation of electrode materials without adhesive.