AbstractWe report a simple, single-cycle synthetic method for forming highly-crystalline, micron-sized monolayer domains of phase-pure MoS₂. This method combines liquid chemistry with discrete, layer-by-layer deposition from a novel Mo precursor. Single-crystalline MoS₂ with domain sizes up to 100 μm have been obtained and characterised by optical and electron microscopy as well as Raman and photoluminescence spectroscopy.