LuLiF 4 single crystals codoped with thulium (Tm) and holmium (Ho) were successfully grown by the Czochralski method. The excellent laser performance, in terms of highest slope efficiency, and highest optical‐to‐optical efficiency and lower laser threshold, was studied in comparison with 5% Tm, 0.5% Ho‐codoped YLiF 4 , and Lu 3 Al 5 O 12 under the same conditions.