Ion beam assisted deposition is a method used to deposit thin films while irradiating the growing film with an ion beam. This technique is known to be effective in crystallization and orientation control at low temperatures. In this study, LiCoO2 (LCO) thin films were prepared at temperatures below 100 °C using ion beam assisted pulsed laser deposition. The structure, composition, and electrochemical properties of these films were characterized. The results indicated that LCO thin films with a disordered rock salt structure and triaxial orientation were successfully grown on polycrystalline aluminum and quartz glass substrates using ion beam assisted deposition. Furthermore, the diffusion coefficient of Li ions and the charge/discharge capacity were significantly improved compared to LCO thin films with a disordered rock salt structure prepared without the ion beam assisted process.