A series of color-tunable green-red-emitting Sr3Y2(Si3O9)(2): Tb3+, Eu3+ (SYSO: Tb3+, Eu3+) were synthesized by solid-state method. The crystal structure and dopant-occupied sites of SYSO: Tb3+, Eu3+ were investigated by XRD-Rietveld refinement. Furthermore, the corresponding luminescent properties were studied in detail. The energy transfer (ET) process from Tb3+ to Eu3+ was found to be resonant type via exchange interaction with ET efficiency of 85%. By varying the Tb3+/Eu3+ ratio, the emitting color can be tuned from green, yellow, orange and eventually to red. The temperature-dependent PL spectra revealed that SYSO: Tb3+, Eu3+ phosphor has good thermal stability. All these properties indicate that the developed phosphor may potentially be used as single-component multicolor-emitting phosphors.