Abstract: The CaxSr1-x-y-zMoO4: yEu³⁺, zNa⁺ as a red phosphor was prepared for LED by solid-state reaction with Na⁺ as charge compensating agents. The effects of Na⁺ dose, Ca²⁺ content in matrix, synthesizing temperature, reaction time and the molecular fraction of Eu³⁺ as luminescent center on the luminescent properties and crystal structure of the phosphor were studied. The results showed that the optimum reaction conditions in molecular fraction are 6% Na⁺, 8% Eu³⁺ and 60% Ca²⁺ with reaction temperature 900 °C for 2 h. The luminescent spectra revealed that the red-emitting phosphor can be effectively excited at 616 nm emitting peak by 311 nm, 395 nm or 465 nm.