A highly crystalline single- or few-layered 2D-MoS2 induces a high dark current, due to which an extremely small photocurrent generated by a few photons can be veiled or distorted. In this report, we show that suppression in the dark current with the enhancement in the photocurrent of a 2D-based photodetector, which is a prerequisite for photoresponse enhancement, can be achieved by constructing an ideal p‐n junction based on functionalizing n-type 2D-MoS2 with p-type quantum dots (QDs). Highly crystalline solution-processed manganese oxide QDs (MnO QDs) are synthesized via the pulsed femtosecond laser ablation technique in ethanol. The ablated MnO QDs are spray-coated on an exfoliated 2D-MoS2 substrate with interdigitated Au electrodes through N2-assisted spraying. In the resulting MnO QD-decorated 2D-MoS2 photodetector with a heterojunction, dark current is reduced and is accompanied by …