This work presents the ultraviolet–visible spectroscopic properties of Ba3Y2(BO3)4:Ce3+,Tb3+ phosphors prepared by a high-temperature solid-state reaction. Under ultraviolet light excitation, tunable emission from the blue to yellowish-green region was obtained by changing the doping concentration of Tb3+ when the content of Ce3+ is fixed. The efficient energy transfer process between Ce3+ and Tb3+ ions was observed and confirmed in terms of corresponding excitation and emission spectra. In addition, the energy transfer mechanism between Ce3+ and Tb3+ was proved to be dipole–dipole interaction in Ba3Y2(BO3)4:Ce3+,Tb3+ phosphor. By utilizing the principle of energy transfer and appropriate tuning of Ce3+/Tb3+ contents, Ba3Y(BO3)4:Ce3+,Tb3+ phosphors can have potential application as an UV-convertible phosphor for near-UV excited white light-emitting diodes.