A novel hole transport layer (HTL) composed of ultrathin two-dimensional, molybdenum disulfide (MoS 2 ) sheets decorated with 20 nm gold nanoparticles (NPs) (MoS 2 @Au) was developed to make use of plasmonics for organic solar cells (OSCs). Both experimental and theoretical simulations revealed that the device with the MoS 2 @Au composite as the HTL exhibited enhanced short-circuit photocurrent density (J sc ) and efficiency compared to that with MoS 2 alone as the HTL.The employment of light trapping based on the localized surface plasmon resonance (LSPR) effect of metallic nanostructures has proven to be a promising strategy to improve light harvesting for organic solar cells (OSCs). 1-3 Such efficient light trapping and coupling strategies achieve the balance between charge transport and light absorption required to improve the efficiency of thin lm photovoltaics. 4 Metallic nanoparticles (NPs) are the most widely utilized sub-wavelength antennas for two primary reasons. 5-9 Firstly, the plasmonic near-eld can be coupled with the adjacent photoactive materials to effectively increase the cross-section of absorption. Secondly, metallic NPs can also be used as sub-wavelength scattering elements to prolong the optical path of the incident light within the photoactive layer. 1 We have previously shown that large-sized, metallic NPs can reect and scatter light better than smaller ones. 10-12 However, small-sized NPs (i.e., <50 nm) are a much better choice because of the ultra-thin layers of the OSC devices. 13 For these small-sized NPs, enhanced light trapping is mainly contributed by plasmonic near-eld enhancement instead of by plasmonic scattering effects. 14 Because the spatial arrangement of the enhanced optical absorption is conned to the area close to the metal surface, 1 the most straightforward and efficient way to achieve enhancement is to place metallic NPs in the photoactive layer 15-18 where the neareld enhancement of electromagnetic elds from the LSPR generates enhanced light absorption in the active materials surrounding the NPs. Nevertheless, in this approach, the possibility of carrier recombination and exciton quenching between the active materials and the metallic NPs through the non-radiative energy transfer may also increase. 17,19,20 In addition, the incorporation of NPs into the active layer may induce the formation of unfavorable lm morphologies and disturb the donor-acceptor phase distribution, depressing the exciton separation and charge collection. 15,16 As a result, even though there are numerous methods to successfully embed metallic NPs in the interfacial layers [e.g., poly(3,4-ethylenedioxy-thiophene):poly(styrenesulfonate) (PEDOT:PSS)] adjacent to the photoactive layers, 21-25 the direct incorporation of plasmonic NPs into the bulk-heterojunction (BHJ) layer of OSC devices remains an urgent challenge.Very recently, chemically-exfoliated molybdenum disulde (MoS 2 ) has been reported to be a novel hole transport material with the potential to replace traditional PEDOT:PSS in ...