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Abstract Monolayer MoS2 has shown excellent photoresponse properties, but its promising applications in high-sensitivity photodetection suffer from the atomic-thickness-limited adsorption and band gap-limited spectral selectivity. Here we have carried out investigations on MoS2 monolayer-based photodetectors with and without decoration of ZnO quantum dots (ZnO-QDs) for comparison. Compared with monolayer MoS2 photodetectors, the monolayer ZnO-QDs/MoS2 hybrid device exhibits faster response speed (1.5 s and 1.1 s, respectively), extended broadband photoresponse range (deep UV-visible), and enhanced photoresponse in visible spectrum, such as higher responsivity over 0.084 A/W and larger detectivity of 1.05 × 1011 Jones, which results from considerable injection of carries from ZnO-QDs to MoS2 due to the formation of I-type heterostructure existing in the contact interface of them.