Here, we explore the use of 2D materials in functional, 3D systems formed via geometry transformation guided by compressive buckling, with a focus examples in constructs that provide 3D photodetection/imaging capabilities by use of light sensing elements that incorporate monolayer MoS2 and graphene, each of which offers an extraordinary combination of electrical, mechanical and optical properties relevant for present purposes. Specifically, graphene offers the best set of parameters for flexible, transparent conductors, with potential to replace indium–tin–oxide in flat panel displays and touch screens22,23. Additionally, MoS2 is of great interest for its excellent semiconducting properties at atomic thicknesses24–26. Owing to a direct band gap of 1.9 eV in monolayer MoS2, this material is well-suited for applications in the unique photodetecting systems27–32. Realizing 3D arrays of MoS2/graphene photodetectors involves first optimizing the parameters for assembly of origami-inspired 3D shapes (an octagonal prism, an octagonal prismoid, and a hemisphere) using finite-element analysis (FEA). The set of assembly parameters defined in this way serves as starting points for experimentally constructing the targeted 3D shapes, with integrated devices, by compressive buckling. Here, MoS2 and graphene serve as the channel and electrodes, respectively, in ultrathin semiconductor photoresistor supported by a layer of polymer. The resulting system forms spontaneously, and without external application of targeted forces, from a 2D planar geometry into a 3D configuration that allows tracking of both the direction and intensity of incident light. As an additional feature, the atomically thin MoS2 and graphene yield optically transparent devices, such that light passing through the device can be detected at two sensing locations (the entry and exit sites), thereby providing further information of relevance to divergence angle.