Synthesizing transition metal dichalcogenide (TMDC) mono layers through the liquid exfoliation of bulk crystals in low boiling point polar micromolecular solvents, such as water, is paramount for their practical application. However, the resulting hydrodynamic forces only appear on the crystal edges due to the mismatch in surface tension between the polar micromolecular solvents and the bulk crystals and are insufficient to overcome the strong van der Waals attraction between adjacent microscale layers. Herein, we present the novel strategy of engineering the lateral size of TMDC (MoS2 and WS2) crystals in the nanoscale to increase the fraction of edges, leading to their direct and ready exfoliation in polar micromolecular solvents, even in pure water, to produce monolayer MoS2 and WS2 nanosheets in high yield. To examine one of their important applications, their catalytic hydrogen evolution activities were evaluated when used as cocatalysts with a photoharvester semiconductor (cadmium sulfide, CdS) in a reaction driven by solar energy. These exfoliated MoS2 (WS2) monolayers exhibited superior cocatalytic performance in the photocatalytic hydrogen evolution reaction (HER). Notably, the cocatalytic performance of monolayer WS2 nanosheets is even higher than that of platinum (Pt), which is a state-of-the-art catalyst for catalytic hydrogen evolution. This work elucidates the importance of decreasing the lateral size of layered crystals to significantly enhance their exfoliability, providing a new strategy for the large-scale preparation of nanoscale TMDC monolayers by liquid exfoliation.