Stimuli responsive self-folding structures with 2D layered materials (2DLMs) are

important for flexible electronics, wearables, biosensors, bioelectronics, and

photonics. Previously, strategies have been developed to self-fold 2D materials to

form various robots, sensors, and actuators. Still, there are limitations with

scalability and a lack of design tools to obtain complex structures for reversible

actuation, high integration, and reliable function. Herein, a mass-producible

strategy for creating monolayer graphene-based reversible self-folding structures

using either gradient or differentially cross-linked films of a negative epoxy

photoresist widely used in microfluidics and micromechanical systems, namely,

SU8 is demonstrated. Wafer-scale patterning and integration of complex and

functional devices in the form of rings, polyhedra, flowers, and bidirectionally

folded origami birds are achieved. Also, gold (Au) electrodes to realize functional

graphene–Au Schottky interfaces with enhanced photoresponse and 3D angle

sensitive detection are integrated. The experiments are guided and rationalized by

theoretical methods including coarse-grained models, specifically developed for

the tunable mechanics of this photoresist that simulate the folding dynamics, and

finite element method (FEM) electromagnetic simulations. This work suggests

a comprehensive framework for the rational design and scalable fabrication of

complex 3D self-actuating optical and electronic devices through the folding of

2D monolayer graphene.