EuM2S4 (M = Ga, Al) phosphors were synthesized using the solid-state reaction method. The structure and photoluminescence (PL) properties of the phosphors were investigated in detail. XRD pattern results indicated that the two phosphors are isostructures to the orthorhombic structure. The PL spectra showed that the EuGa2S4 and EuAl2S4 phosphors can be excited efficiently by UV–visible light from 350 to 480 nm and that they emit intense green and bluish-green light, with emission bands peaking at 545 and 506 nm, respectively. The fluorescence lifetimes of Eu2+ were calculated to be 0.076 and 0.064 µs for EuGa2S4 and EuAl2S4, respectively. The thermal quenching temperature was 412 K for EuGa2S4. A green LED was fabricated by the combination of a near-UV InGaN chip and the prepared EuGa2S4 phosphor. The EuGa2S4 phosphor exhibits much better green color purity than EuAl2S4. As a result, EuGa2S4 might be a promising green phosphor candidate for solid-state lighting LED technology.