Polycrystalline Gd2(MoO4)3:Dy3+ phosphors have been synthesized by high temperature solid-state reaction method. The phosphors were characterized with X-ray diffractometer, thermogravimetric analysis and different scanning calorimeter, scanning electron microscopy, and photoluminescence spectrofluorimeter. Several peaks at 351, 389, 425, 452, and 472 nm appeared in photoluminescence excitation spectrum, which matched well with the emission of the ultraviolet (UV) and blue-light emitting diode (LED) chips. Upon excitation at 389 nm UV light, intense emissions centered at 484, 575 and 668 nm were attributed to the transitions of 4F9/2→6H15/2, 4F9/2→6H13/2 and 4F9/2→6H11/2 of Dy3+, respectively. The chromaticity coordinates and correlative color temperatures have been calculated and presented in the Commission International de I’Eclairage (CIE) diagrams. The results indicated that Gd1.9(MoO4)3:Dy0.13+ with CIE coordinates of (x=0.38, y=0.41) and the correlative color temperature of 4134 K is a potential candidate for white LEDs.