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The microstructure and photoluminescence properties of Gd0.94-xAlxEu0.06VO4 (0≤x≤0.04) phosphors with various Al3+ contents were investigated. The phosphors showed a nanocrystalline nature and a high-quality powder characteristic. The crystallite sizes of the phosphors were calculated to be 46-48 nm. The annealed Gd0.94-xAlxEu0.06VO4 phosphors crystallized in the tetragonal structure. In the emission spectra, several emission peaks were observed over the measured wavelength range (500-750 nm), which were caused by the difference in the transitions of Eu3+ ions, depending on the local symmetry (5D0 → 7Fj, j = 1, 2, 3, and 4). The strongest emission peak was located at 619 nm, providing a high-purity red emission. The doped Al3+ yielded significantly enhanced the emission intensity. The most intense high-purity red emission was obtained for Gd0.93Al0.01Eu0.06VO4.