Buckling and wrinkling of thin films on a compliant material has proved to be a resource in several applications, such as flexible electronics, thin‐film metrology and fabrication of tunable optical components. A versatile approach for the fabrication of two‐dimensional and linear arrays of buckled structures is demonstrated here using a stiff material, in the form of a nanomembrane, on a compliant substrate. The novelty of the fabrication process is that the substrates are strained by isotropic volume expansion in solvents. This work illustrates in detail the potential of our technology to fabricate ordered arrays of 3D structures on large‐area compliant substrates, with important implications for a large number of fields. Furthermore, this paper discusses the interesting interface chemistry and mechanics leading to controllable and reproducible fabrication of our 3D structures.
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