One-pot hydrothermal synthesis of MoS2 nanoplatelet arrays on various substrates is perhaps the most promising approach to fabricate efficient electrocatalysts for hydrogen evolution reaction. However, the main challenges in this synthesis remain the purity and crystallinity of MoS2. In this study, we show for the first time that irradiation of amorphous, defect-rich MoS2 nanoplatelets with a green nanosecond laser at a proper irradiation dose, ca ≤0.35 J cm-2, can significantly improve the crystallinity and purity of MoS2 nanoplatelets. The effect was confirmed by Raman spectroscopy investigations demonstrating a surprising intensity increase of the A1g and modes after the laser irradiation. Further increase of irradiation energy, however, resulted in the photocorrosion and destruction of MoS2 nanoplatelets. The variation of A1g and Raman mode intensities ratio depending on the green light irradiation dose was also presented and is discussed below.