Origami is a topic of rapidly growing interest in both the scientific and engineering research communities due to its promising potential in a broad range of applications. Previous assembly approaches for origami structures at the micro/nanoscale are constrained by the applicable classes of materials, topologies, and/or capability for reversible control over the transformation process. Here, a strategy is introduced that exploits mechanical buckling for autonomic origami assembly of 3D structures across material classes from soft polymers to brittle inorganic semiconductors, and length scales from nanometers to centimeters. This approach relies on a spatial variation of thickness in the initial 2D structures as a means to produce engineered...