has attracted much attention and been extensively studied as the transistor [7] or photodetector devices. [8,9] However, the absorption of the incident light may be limited from the reduced atomic thickness of the MoS 2 . Meanwhile, plasmonic materials, especially the noble metals (e.g., platinum and gold), have been reported to facilitate the strong light-matter interaction and carrier transportation at the intimate interface of semiconductor-metal nanodomains. [10,11] Previous works have revealed the enhanced electromagnetic field and the light confinement effect by combining plasmonic metal nanostructures and 2D-based photodetectors, leading to the improvement of the light absorption under the visible spectral region. [12][13][14][15] Also, by applying metal particles with diverse morphologies such as nanoparticles, [16][17][18][19] nanotubes/ nanowires, [20,21] nanodiscs, [22][23][24] core-shell particles [25,26] and creating nanoarray patterns, [27][28][29] the resonance wavelength can be tunable. To achieve the better performance of photodetector on the MoS 2 layered material, we aim to combine highly absorptive CuInS 2 (CIS) nanoparticles with noble metal nanoparticles as the photosensitizer to enhance the intrinsic absorptivity of noble metal nanocrystals. The interests of noble nanocrystals such as platinum and gold are featured for their distinctive properties of the carrier transportation and the storage when combined with semiconductor materials. [30,31] The accompanying noble metal NPs induce an A facile approach for the synthesis of Au-and Pt-decorated CuInS 2 nanocrystals (CIS NCs) as sensitizer materials on the top of MoS 2 bilayers is demonstrated. A single surfactant (oleylamine) is used to prepare such heterostructured noble metal decorated CIS NCs from the pristine CIS. Such a feasible way to synthesize heterostructured noble metal decorated CIS NCs from the single surfactant can stimulate the development of the functionalized heterostructured NCs in large scale for practical applications such as solar cells and photodetectors. Photodetectors based on MoS 2 bilayers with the synthesized nanocrystals display enhanced photocurrent, almost 20-40 times higher responsivity and the On/Off ratio is enlarged one order of magnitude compared with the pristine MoS 2 bilayers-based photodetectors. Remarkably, by using Pt-or Au-decorated CIS NCs, the photocurrent enhancement of MoS 2 photodetectors can be tuned between blue (405 nm) to green (532 nm). The strategy described here acts as a perspective to significantly improve the performance of MoS 2 -based photodetectors with the controllable absorption wavelengths in the visible light range, showing the feasibility of the possible color detection.