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Wide bandgap β-Ga2O3 is an ideal candidate material with broad application prospects for power electronic components in the future. Aiming at the application requirements of β-Ga2O3 in space photoelectric devices, this work studies the influence of 40 MeV Si ion irradiation on the microstructure and optical properties of β-Ga2O3 epi-wafers. Raman spectroscopy analysis confirms that Si ion irradiation destroys the symmetric stretching mode of tetrahedral–octahedral chains in β-Ga2O3 epi-wafers, and the obtained experimental evidence of irradiation leads to the enhanced defect density of VO and VGa–VO from x-ray photoelectron spectroscopy. Combined with first-principles calculations, we conclude that most configurations of VO and VGa–VO are likely non-radiative, leading to quenching of experimental photoluminescence intensity. Unraveling optical degradation mechanism and predicting the optical application of β-Ga2O3 devices in the space environment by combining ground irradiation experiments with first-principles calculations still be one of the focuses of research in the future. [ABSTRACT FROM AUTHOR]