Scheelite related alkali-metal rare-earth double molybdate compounds with a general formula of ALn(MoO4)2 can find wide application as red phosphors. The crystal chemistry and luminescence properties of red-emitting CsGd1-xEux(MoO4)2 solid-solution phosphors have been evaluated in the present paper. A detailed analysis of the structural properties indicates the formation of isostructural scheelite-type CsGd1-xEux(MoO4)2 solid-solutions over the composition range of 0 ≤ x ≤ 1. The photoluminescence emission (PL) and excitation (PLE) spectra, and the decay curves were measured for this series of compounds. The critical doping concentration of Eu(3+) is determined to be x = 0.6 in order to realize the maximum emission intensity. The emission spectra of the as-obtained CsGd(1-x)Eux(MoO4)2 phosphors show narrow high intensity red lines at 592 and 615 nm upon excitation at 394 or 465 nm, revealing great potential for applications in white light-emitting diode devices.