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The photoluminescence (PL) of Al2O3:xCr2O3 solid solutions prepared by solid state reaction were studied. The effects of Cr2O3 activator concentration and heating time on the PL characteristics were investigated in conjunction with microstructural analysis of phosphor samples. Al2O3:xCr2O3 phosphors show the highest PL intensity at x = 0.003 mol when the samples are reacted at 1600 C for 5 h. The PL emission and absorption spectra show maximum peaks at 698 nm and at 398 nm, respectively. The CIE colour coordinate is (x = 0.646, y = 0.316) at 0.003 mol Cr2O3; this value is very close to the NTSC coordinate for red. Al2O3:xCr2O3 was used as an additive to improve the colour of the red phosphor LiEuW2O8, which has a relatively poor colour purity with an emission peak centred at 615 nm and with a CIE coordinate (x = 0.530, y = 0.280). The Al2O3:0.003Cr2O3 phosphor was mixed with LiEuW2O8 phosphor powder, and the PL characteristics and colour coordinates were determined. Al2O3:xCr2O3 phosphor was found to be effective for improving the CRI (colour rendering index) of LiEuW2O8 phosphor.