A passively Q-switched mode-locked (QML) Tm:LiLuF₄ (LLF) laser with a MoS2 saturable absorber (SA) is demonstrated for the first time, to our best knowledge. For the Q-switching mode, the maximum average output power and Q-switched pulse energy are 583 mW and 41.5 μJ, respectively. When the absorbed power is greater than 7.4 W, the passively QML pulse is formed, corresponding to an 83.3-MHz frequency. The modulation depth in Q-switching envelopes is approximately 50%. Results prove that MoS2 is a promising SA for Q-switched and QML solid-state lasers.