First, SU-8 (2 µm) was spin-coated on an SiO2/Si wafer and patterned according to the desired 3D structure (octagonal prism, octagonal prismoid, or hemisphere). After transferring the graphene, the electrodes were defined in an interdigitated geometry by photolithography and reactive ion etching (RIE) with O2 plasma (40 sccm, 100 W, 5 s). MoS2 was transferred onto the interdigitated pattern of graphene electrodes and the channel regions were defined by photolithography and RIE with CHF3/O2 plasma (35/10 sccm) at 100 W for 5 s. Another SU-8 (5 µm) layer was spin-coated and patterned in a manner similar to that for the first SU-8 layer, but with openings in regions designated for creases. PR was spin-coated and patterned to expose and cover the bonding and non-bonding regions, respectively. Assisted by HF treatment, this fabricated structure was transferred with a slab of PDMS to a tape of PVA. Next, an elastomer substrate (Dragon Skin, Smooth-On) was bi-axially pre-stretched to the optimized strain determined by FEA simulations. The structure on the PVA tape and the pre-stretched substrate were exposed to UV ozone, laminated together and then baked in an oven at 70 °C for 5 min. The PVA was then dissolved in DI water. Finally, the PR was dissolved in acetone, which loosened and/or slightly delaminated the non-bonding regions of the devices from the pre-stretched substrate, facilitating the 3D assembly process upon release of the pre-stretching strain. The sizes of MoS2 photoresistor and the 3D pop-up hemisphere structure are 80 × 80 µm and 3.5 × 1.4 mm (diameter × height), respectively. Detailed descriptions of the 3D hemispherical structure and diagrams of the operating principles are in Supplementary Figs. 26 and 27, respectively.