A novel blue-green-emitting phosphor Gd4.67SiO13:Tb3+ has been synthesized by a conventional high temperature solid-state method at 1350 °C for 6 h. X-ray diffraction and photoluminescence spectra were used to characterize the as-synthesized phosphor. The excitation spectrum is composed of a broadband and two sharp peaks, at 274 nm, and 311 nm, respectively. The emission spectrum is composed of multiple sharp peaks, of which the strongest peak is at 544 nm (5D4 -->7F5). The critical doping content of Tb3+ is 5%, with the emission intensity increasing proportionally with Tb3+ concentration increase until it reaches 5%. As doping concentration from 5% to 7%, the luminescence intensity gradually reduces. Concentration quenching mechanism for Tb3+ is demonstrated to be dipole-dipole interaction. The Commission Internationale de L'Eclairage (CIE) coordinates are also investigated in this work. The CIE coordinates of the Gd4.67SiO13:0.03Tb3+ phosphor upon 311 nm excitation are (0.242, 0.323). All the results indicate that the blue-green-emitting phosphor Gd4.67SiO13:Tb3+ has potential research value.