We report the growth, thermal characteristics, and spectroscopic properties of Dy 3+ -doped (Dy:YLF) and Dy 3+ /Tb 3+ codoped LiYF 4 (Dy,Tb:YLF) crystals. The yellow emission at ∼575 nm of the Dy 3+ : 4 F 9/2 → 6 H 13/2 transition of the Dy,Tb:YLF crystal was enhanced by the deactivation effects of codoped Tb 3+ ions. The corresponding ET efficiency from the Dy 3+ : 6 H 13/2 to Tb 3+ : 7 F 4 level was as high as 55.4%, which greatly reduced the energy level lifetime of 6 H 13/2 , and an emission at 575 nm with the emission cross section σ em = 4.58 × 10 −21 cm 2 was obtained, confirming the effective deactivation of Tb 3+ ions, which is beneficial to resolve the self-termination bottleneck effect and achieve enhanced yellow laser emission. Hence, the Dy,Tb:YLF crystal is an attractive and potential laser medium for LD-pumped all-solid-state yellow lasers.