Eu3+-doped transparent phosphate precursor glasses and glass-ceramics containing TbPO4 nanocrystals were successfully fabricated by a conventional high-temperature melt-quenching technique for the first time. The formation of TbPO4 nanocrystals was identified through X-ray diffraction, transmission electron microscopy, high-resolution transmission electron microscopy, selected-area electron diffraction, and photoluminescence emission spectra. The obvious Stark splitting of D-5(0)-F-7(J) (J=1, 2, 4) transitions of Eu(3+)and the increase of internal quantum efficiency indicate the incorporation of Eu3+ into TbPO4 nanocrystals. Energy transfer from Tb3+ ions to Eu3+ ions was investigated using excitation and emission spectra at room temperature. The glass-ceramics obtained have more efficient Tb3+ to Eu3+ energy transfer than the glass, and so serve as good hosts for luminescent materials.