Columnar Gd2O2S:Eu3+ nanophosphors have been synthesized through solvothermal reaction and subsequent calcination process. The structure, morphology, and luminescence properties of samples were investigated via X-ray diffraction (XRD), Fourier transform infra-red (FT-IR) spectra, UV-vis absorption spectra, field emission scanning electron microscope (FE-SEM), and photoluminescence (PL) spectra. The Judd-Ofelt (J-O) parameters of Gd2O2S:Eu3+ nanophosphors with different doping concentration were calculated by emission spectra to understand the symmetry, coordination environment, and luminescence behavior of Eu3+ ions in Gd2O2S matrix. In addition, the luminescence properties of columnar Gd2O2S:Eu3+ and Gd2O3:Eu3+ were compared in detail. The comparison results show that there are subtle differences in luminescence intensity, main peak position, luminescence color, and fluorescence lifetime between them, which are closely related to their different substrate's structure, including the band-gap energy, crystallinity, and symmetry, etc.