LuLiF4 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 YLiF4, and Lu3Al5O12 under the same conditions.