摘要： Recently, asymmetrically functionalized two-dimensional (2D) nanomaterials have attracted fevered interest as excellent candidates for building blocks of multifunctional and multidimensional systems due to the structural symmetry-breaking. However, their preparation process typically involves high vacuum environment or specific equipment, and the obtained samples have poor stability and low yield. In this study, a facile approach has been developed to achieve the asymmetric deposition of platinum nanoparticles (NPs) onto single side of the molybdenum disulfide (MoS2) nanosheets by pyrogenic decomposition and in-situ functionalization. By tuning the platinum precursor to MoS2 ratio, the size distribution and morphology of the Pt NPs can be well controlled. The asymmetrical decoration of Pt NPs on MoS2 nanosheets (Pt-MoS2) may result from the superior interactions between Pt NPs and MoS2 basal surface, which are stronger than the van der Waals force between adjacent MoS2 layers. Hydrogen evolution reaction (HER) results show that higher Pt loading yields better HER performance with low overpotential of 120 mV and superior Tafel slope of 28 mV·dec-1. Significantly, the current synthetic method can be used in the asymmetrical functionalization of other 2D nanosheets as well, and could greatly advance the facile preparation and practical applications of these asymmetric nanostructures.