As is well known, the basic intrinsic properties of materials can be significant for their practical applications. In this work, the room-temperature absorption, transmittance, reflectance spectra, and relative photoelectricities parameters of the Mg4Ta2O9 crystals are demonstrated. Meanwhile, the polarized Raman spectra of Mg4Ta2O9 crystals are also described. The room-temperature photoluminescence (PL) and the temperature-dependent PL for Mg4Ta2O9 crystals are obtained. Significantly, we observe a phonon-participated PL process in Mg4Ta2O9.