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Strong light absorption, coupled with moderate carrier transport properties, makes 2D layered transition metal dichalcogenide semiconductors promising candidates for low intensity photodetection applications. However, the performance of these devices is severely bottlenecked by slow response with persistent photocurrent due to long lived charge trapping, and nonreliable characteristics due to undesirable ambience and substrate effects. Here ultrahigh specific detectivity ( D *) of 3.2 × 10 14  Jones and responsivity ( R ) of 5.77 × 10 4  A W −1  are demonstrated at an optical power density ( P  op ) of 0.26 W m −2  and external bias ( V  ext ) of −0.5 V in an indium tin oxide/MoS 2 /copper oxide/Au vertical multi‐heterojunction photodetector exhibiting small carrier transit time. The active MoS 2  layer being encapsulated by carrier collection layers allows us to achieve repeatable characteristics over large number of cycles with negligible trap assisted persistent photocurrent. A large  D * > 10 14  Jones at zero external bias is also achieved due to the built‐in field of the asymmetric photodetector. Benchmarking the performance against existing reports in literature shows a viable pathway for achieving reliable and highly sensitive photodetectors for ultralow intensity photodetection applications.

Asymmetrically Encapsulated Vertical ITO/MoS 2 /Cu 2 O Photodetector with Ultrahigh Sensitivity