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In this work, we systematically study the spectroscopic properties of Tb3+/Dy3+ co‐doped phosphate glasses in the visible spectral region and explore the sensitization role of Dy3+ in the enhancement of visible fluorescence of Tb3+ ions. Judd‐Ofelt parameters Ω2 and Ω4/Ω6 of the phosphate glass as host for Tb3+ are calculated as 21.60 × 10‐20 cm2 and 0.73, respectively, based on the measured spectral absorption. Multiple energy transfer (ET) routes from Dy3+ to Tb3+ and their efficiencies are characterized, and the enhanced fluorescence properties of Tb3+ are investigated, including the emission spectral strength and the spontaneous emission lifetime as functions of Dy3+ doping concentration. The efficient nonradiative ET processes between Dy3+ and Tb3+ allow a moderate concentration level of Tb3+ to achieve favorably stronger spectral absorption at blue and ultraviolet wavelengths. Tb3+/Dy3+ co‐doped phosphate glass shows promising potential for phosphors and lasing operation at visible wavelengths. [ABSTRACT FROM AUTHOR]