This Perspective focuses on the design of hierarchical structures in deformable thin materials by patterning mechanical instabilities. Fabrication of three-dimensional (3D) structures with multiple length scales-starting at the nanoscale-can result in on-demand surface functionalities from the modification of the mechanical, chemical, and optical properties of materials. Conventional top-down lithography, however, cannot achieve 3D patterns over large areas (>cm2). In contrast, a bottom-up approach based on controlling strain in layered nanomaterials conformally coated on polymeric substrates can produce multiscale structures in parallel. In-plane and out-of-plane structural hierarchies formed by conformal buckling show unique structure-function relationships. Programmable hierarchical surfaces offer prospects to tune global- and local-level characteristics of nanomaterials that will positively impact applications in nanomechanics, nanoelectronics, and nanophotonics.