M2SiO4: Tb3+, Mn2+, Nd3+ (M = Mg2+, Ca2+, Sr2+, and Ba2+) phosphors suitable for near-ultraviolet-violet radiation excitation were successfully prepared at 1400 °C in N2 atmosphere by a high-temperature solid-state reaction, and their phase compositions and luminescent performance were also studied by X-ray diffraction (XRD), photoluminescence spectra. Results show that their emission intensity increases in the order of Ca2SiO4 > Mg2SiO4 > Sr2SiO4 > Ba2SiO4 matrix phosphor. Ca1.94SiO4: 0.02Tb3 +, 0.02Mn2+, 0.02Nd2+ phosphor exhibits the best luminescence performance.