A series of phosphors Ca3La3(1-x)Tb3x(BO3)5 were synthesized by using a high-temperature solid-state reaction technique, and their VUV-vis luminescence properties were investigated. Strong host-related absorption is observed in the VUV region, and the f–d transitions of Tb3+ in the host lattice are assigned and discussed. The influence of both the doping concentration and the temperature on the spectroscopic properties that include the relative emission intensity and the decay time is investigated.