Sandwich-like molybdenum sulfide/mesoporous organosilica nanosheets (denoted as MoS2@MOS) have been prepared for the first time via direct growth of ethane-bridged mesostructured organosilica on MoS2 nanosheets by using cetyltrimethylammonium bromide (CTAB) as structure directing agent. The obtained MoS2@MOS nanosheets possess well-defined sandwich-like structure, high surface area (∼920cm2/g), uniform pore size (∼4.2nm), large pore volume (∼1.41cm3g−1). In vitro cytotoxicity assessments demonstrate that the MoS2@MOS nanosheets have excellent biocompatibility. Owing to the encapsulation of the MoS2, the obtained MoS2@MOS nanosheets have photo-thermal conversion capability and photo-thermally controlled drug release property. These properties make the MoS2@MOS nanosheets promising for biomedical applications.