Microassembly based on origami, the Japanese art of paper folding, presents an attractive methodology for constructing complex three-dimensional (3D) devices and advanced materials. A variety of functional structures have been created using patterned metallic, semiconducting, and polymeric thin films, but have been limited to those that curve in a single direction. We report a design framework that can be used to achieve spontaneous bidirectional folds with any desired angle, and we demonstrate theoretical and experimental realizations of complex 3D structures with +90°, −90°, +180°, and −180° folds. The strategy is parallel, versatile, and compatible with conventional microfabrication.

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