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Abstract A photocrosslinkable poly(N,N′‐diethylacrylamide) copolymer allows for the photolithographic fabrication of hydrogel sheets with nonuniform crosslinking density and swelling ratio. Using this material system, different 3D shapes with nonzero Gaussian curvatureKare successfully programmed by prescribing a “metric” defined by in‐plane variations in swelling. However, this methodology does not control the direction of buckling adopted by each positive K feature, and therefore cannot controllably select between different isometric shapes defined by a single metric. Here, by introducing gradients in swelling through the thickness of the gel sheet by tuning the absorption of the UV‐light used for crosslinking, a preferential buckling direction is locally specified for each feature by the direction of UV exposure. By also controlling the strength of coupling between neighboring features, this is shown to be an effective method to program buckling direction of each unit within a canonical corrugated surface shape. 

Abstract Self‐folding is a powerful approach to fabricate materials with complex 3D forms and advanced properties using planar patterning steps, but suffers from intrinsic limitations in robustness due to the highly bifurcated nature of configuration space around the flat state. Here, a simple mechanism is introduced to achieve robust self‐folding of microscale origami by separating actuation into two discrete steps using different thermally responsive hydrogels. First, the vertices are pre‐biased to move in the desired direction from the flat state by selectively swelling one of the two hydrogels at high temperature. Subsequently, the creases are folded toward their target angles by activating swelling of the second hydrogel upon cooling to room temperature. Since each vertex can be individually programmed to move upward or downward, it is possible to robustly select the desired branch even in multi‐vertex structures with reasonably high complexity. This strategy provides key new principles for designing shaping‐morphing materials that avoid undesired distractor states, expanding their potential applications in areas such as soft robotics, sensors, mechanical metamaterials, and deployable devices.