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High‐optical‐quality ternary [(Y1‐xGdx)0.99Dy0.01]2O3 (x = 0 and 0.4) ceramics were successfully fabricated by vacuum sintering with in‐line transmittances of 71.4%‐75.1% at 574 nm, the wavelength of Dy3+ emission (the 4F9/2 → 6H13/2 transition). Substitution of Gd3+ for Y3+ significantly affected the photoluminescent and scintillant properties of the ceramics. Gd3+ addition effectively increased lattice parameters and theoretical densities of the ceramic samples; this contributed to enhanced X‐ray absorption coefficients. Both [(Y1‐xGdx)0.99Dy0.01]2O3 (x = 0 and 0.4) ceramics displayed typical Dy3+ emissions from 4F9/2 → 6HJ (J = 15/2, 13/2, 11/2) transitions under UV and X‐ray irradiations. By incorporating Gd3+ into the lattice, a stronger excitation peak of Gd3+ due to internal f‐f transitions relative to Dy3+ was observed at 276 nm; subsequent ceramics obtained a sharper PL intensity and a warmer hue via effective energy transfer from Gd3+ to Dy3+. Using a Gd3+ dopant generally reduces the total photoluminescence/photoluminescence excitation intensities and light output; it also delays the lifetime and afterglow of the transparent ceramics. [ABSTRACT FROM AUTHOR]