We fabricated dye-sensitized MoS2 photodetectors that utilized a single-layer MoS2 treated with rhodamine 6G (R6G) organic dye molecules (with an optical band gap of 2.38 eV or 521 nm). The proposed photodetector showed an enhanced performance with a broad spectral photoresponse and a high photoresponsivity compared with the properties of the pristine MoS2 photodetectors. The R6G dye molecules deposited onto the MoS2 layer increased the photocurrent by an order of magnitude due to charge transfer of the photoexcited electrons from the R6G molecules to the MoS2 layer. Importantly, the photodetection response extended to the infrared (λ < 980 nm, which corresponded to about half the energy band gap of MoS2), thereby distinguishing the device performance from that of a pristine MoS2 device, in which detection was only possible at wavelengths shorter than the band gap of MoS2, i.e., λ < 681 nm. The resulting device exhibited a maximum photoresponsivity of 1.17 AW(–1), a photodetectivity of 1.5 × 10(7) Jones, and a total effective quantum efficiency (EQE) of 280% at 520 nm. The device design described here presents a significant step toward high-performance 2D nanomaterial-based photodetector.