The novel phosphors of LaAlGe 2 O 7 doped with Gd 3+ and Tb 3+ were synthesized, and their luminescence properties were investigated. In Tb 3+ -activated LaAlGe 2 O 7 , the unusual excitation spectra showed only intense f-f transition of Tb 3+ ions around the near-UV region, whereas the 4f-5d transition could be neglected. In the Gd 3+ -Tb 3+ -activated system, the decay time of Tb 3+ emission under Gd 3+ excitation at the 6 I J energy level was longer than that measured under direct Tb 3+ excitation at the 5 L 10 energy level, which reinforces the existence of effective Gd 3+ -to-Tb 3+ energy transfer. In the 5 D 4 decay measurements, time-resolved spectra exhibited a "grow-in" behavior as the Tb 3+ concentration was diluted (<0.03 mol), whereas only a simple exponential decay could be observed at higher (>0.05 mol) Tb 3+ concentrations. Two linear relationships were found between the energy transfer probability (P GdfTb ) and the Tb 3+ concentration, which is clear evidence that there were two kinds of efficient Gd 3+ -to-Tb 3+ energy transfer processes in terms of Tb 3+ concentration.