This paper reported the fabrication of high-performance ZnIn2S4 photocatalysts using ionic liquid microemulsion-mediated hydrothermal method under facile conditions. The influences of reaction temperature and aging time on the catalytic properties of the specimens were investigated. The crystal phase, optical property, and morphological structure of the obtained catalysts were characterized using X-ray diffraction, UV-visible spectrometer, electronic microscope, and N-2 adsorption-desorption techniques. The results indicated that all of the ZnIn2S4 samples prepared by this method consisted of the hexagonal phase and exhibited excellent photoresponse capability and photocatalytic performance. The sample prepared at 60 A degrees C with an aging time of 6 h showed the best photocatalytic performance, and the corresponding degradation rate of methyl orange was measured as 98.5% after 10 min. The current study highlights an efficient and environmental method for the formulation of high-performance ZnIn2S4.