Conventional photolithography is an effective patterning technique that has enabled modern electronics and advanced micro- and nanoscale devices. However, it has limitations, including high cost, limited resolution, and poor compatibility with unconventional materials that may be soft, nonplanar, or difficult to process. There is active research ongoing to develop unconventional patterning methods such as self-organization and self-folding. Self-organization harnesses various driving forces to produce patterns without external intervention and includes methods such as self-assembly of block copolymers, capillary-driven assembly of micro-/nanoscale structures, and thin-film instabilities. Self-folding (origami)—and its cousin, kirigami—harnesses patterning and materials strategies to convert planar substrates into three-dimensional shapes in response to external stimuli. These multidisciplinary approaches open many engineering opportunities by providing new and versatile material functionalities. This article overviews the field and the topics covered in the articles in this issue of MRS Bulletin, highlighting recent progress in patterning approaches based on self-organization and self-folding.