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As an emerging two-dimensional (2D) nanomaterial, single layer or a few layers of molybdenum disulfide (MoS2) has drawn significant attention in the past decade. In the present work, we report a strategy in direct creating polymer brushes on MoS2 surfaces via S-C bond in the presence of UV light. The modification of MoS2 nanosheets can be achieved bilaterally or homolaterally by performing the UV grafting polymerization on exfoliated MoS2 nanosheets or a single layer of MoS2 deposited on a silicon substrate. A series of vinyl monomers including methyl methacrylate (MMA), styrene (St) and 2-isopropenyl-2-oxazoline (IPOx) could be applied to this approach, leading to the formation of poly (methyl methacrylate) (PMMA), polystyrene (PS) and poly(2-isopropenyl-2-oxazoline) (PIPOx) brushes. AFM, IR, and XPS characterizations indicate the successful formation of homogeneous brush layers on MoS2 surfaces. The polymer brushes modified MoS2 may found potential applications in photo dynamic therapy and sensing technologies.