A series of color tunable Tb3+- and Eu3+-activated Sr2P2O7 phosphors were synthesized by a traditional solid-state reaction method in air atmosphere. The crystal structure, photoluminescence (PL) properties, energy transfer, thermal stability, and luminous efficiency were investigated. A series of characteristic emission of Tb3+ and Eu3+ were observed in the PL spectra and the variation in the emission intensities of the three emission peaks at around 416 nm (blue), 545 nm (green), and 593 nm (orange-red) induced the multicolor emission evolution by tuning the Tb3+/Eu3+ content ratio. The energy-transfer mechanism from Tb3+ to Eu3+ ion was determined to be dipole-dipole interaction, and the energy-transfer efficiency was about 90%. The novel phosphors have excellent thermal stability in the temperature range of 77-473 K and the Commission International De L'Eclairage 1931 chromaticity coordinates of Sr2P2O7: Tb3+, Eu3+ (lambda(ex) = 378 nm) move toward the ideal white light coordinates.