In this work, a facile chemical route is presented to prepare photoluminescent MoS2 quantum dots (QDs) and nanosheets (NSs) on a large‐scale. The strategy involves probe‐type sonication of bulk MoS2 sheets in ethanol/water mixture followed by refluxing in dimethylformamide (DMF) solution. This preparation route makes cleavage of the Van‐der‐Waal layers possible by exfoliation across the 2D planes and the complete breakup of bulk MoS2 sheets around the defects and edges. The as‐prepared MoS2 QDs and NSs exhibit size quantization effects in their optical absorption and emission spectra. The resultant MoS2 NSs consist of few layers with lateral size around ∼80 nm and exhibit excitation dependent blue emission. Whereas, most of the MoS2 QDs were measured around ∼4.8 nm in lateral size and showed distinct green emission upon excitation. This may be attributed to a combined contribution from the increase in the quantum‐sized core, edge defects, dangling bonds, and surface states recombination. The study thus provides a simple pathway for the preparation of monolayer QDs and few‐layer NSs of transition‐metal‐dichalcogenides (TMD) or other layered materials.