Broad-band near-ultraviolet (NUV)-excited and multicolor-emitting Gd2SiO5:Ce3+,Tb3+,Eu3+ phosphors were synthesized by solid-state reaction. The emission color of the phosphors can be tuned from blue (0.153, 0.091) to green (0.325, 0.495) and eventually to red (0595, 0.370) through efficient Ce3+ -> (Tb3+)(n) -> Eu3+ energy transfer. NUV light was strongly absorbed by the Ce3+ ions, and the excited energy was transferred to Tb3+ ions, which produced intense green emission peaks. Finally, the excited energy was transferred from Tb3+ to Eu3+ ions, which is attributed to red emission peaks. These multicolor tunable Gd2SiO5:Ce3+,Tb3+,Eu3+ phosphors are promising materials for applications in NUV light-emitting diodes.