that offers novel electrical, electronic, and optical properties that are distinct from their bulk counterparts along with mechanical flexibility and high compatibility with state-of-the-art silicon-based platform. [2][3][4] Among prominently studied materials in the last few decades is zinc oxide (ZnO), a highly versatile tunable material. [5] The optoelectronic properties of ZnO in various morphologies have been investigated widely. [6] Due to its strong absorption in the UV region, ZnO is an attractive candidate for visible-blind photodetectors. [7] With a wide bandgap of 3.39 eV, exciton binding energy as large as 60 meV at room temperature, and the ability to undergo a strong quantum confinement effect, atomically thin ZnO promises an excellent platform for optoelectronic applications. [8] Most importantly, oxygen adsorbed onto the surface of ZnO provides low electron densities that can enable low dark current which is ideal for low energy applications. [9] Though thin nanosheets (<20 nm) ZnO has been used as an active layer for various applications, the lack of a reliable and controllable synthesis technique to obtain large area few atoms thin ZnO has prevented the miniaturization of ZnO based optoelectronic devices slowly making the material less competitive compared to other emerging systems relying on atomically thin functional layers. [10][11][12] Also, ZnO and other planar metal-semiconductormetal (MSM) based UV photodetectors developed to date have Atomically thin 2D materials are highly sought for high-performance electronic and optoelectronic devices. Despite being a widely recognized functional material for a plethora of applications, ultra-thin nanosheets of zinc oxide (ZnO) at a millimeter-scale for developing high-performance electronic/optoelectronic devices have not been reported. This has prevented the exploration of electronic and optical properties of ZnO when it is only a few atoms thick. Here, a liquid metal exfoliation technique is used that takes advantage of the van der Waals forces between the interfacial oxide and the chosen substrate to obtain ZnO nanosheets with lateral dimensions in the millimeter scale and thickness down to 5 nm. Their suitability for applications is shown by demonstrating a visible-blind photodetector with high figures of merit as compared to other ZnO morphologies. At extremely low operating bias of 50 mV and low optical intensity of 0.5 mW cm −2 , the ZnO photodetector demonstrates an external quantum efficiency (EQE), responsivity (R), and detectivity (D*) of 4.3 × 10 3 %, 12.64 A W −1 , and 5.81 × 10 15 Jones at a wavelength of 365 nm. The trap-mediated photoresponse in the ZnO nanosheets is further utilized to demonstrate optoelectronic synapses. Versatile synaptic functions of the nervous systems are optically emulated with the ultra-thin ZnO nanosheets.