We report on the high average power third harmonic generation (THG) of a mode-locked picosecond laser in a CsB3O5 (CBO) crystal. The picosecond laser beam at 1064 nm is produced by a home-made 30 W master oscillator power-amplifier (MOPA) Nd:YVO4 laser system. The maximum THG output at 355 nm is up to 5.4 W. We also investigate the phase matching angle at different temperatures. During high power operation, the temperature of the CBO crystal is set at a high temperature of more than 100 °C. The THG system has shown a fine long-term stability for more than two months of operation.