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Formation of 3D mesostructures in advanced functional materials is of growing interest due to the widespread envisioned applications of devices that exploit 3D architectures. Mechanically guided assembly based on compressive buckling of 2D precursors represents a promising method, with applicability to a diverse set of geometries and materials, including inorganic semiconductors, metals, polymers, and their heterogeneous combinations. This paper introduces ideas that extend the levels of control and the range of 3D layouts that are achievable in this manner. Here, thin, patterned layers with well-defined residual stresses influence the process of 2D to 3D geometric transformation. Systematic studies through combined analytical modeling, numerical simulations, and experimental observations demonstrate the effectiveness of the proposed strategy through ≈20 example cases with a broad range of complex 3D topologies. The results elucidate the ability of these stressed layers to alter the energy landscape associated with the transformation process and, specifically, the energy barriers that separate different stable modes in the final 3D configurations. A demonstration in a mechanically tunable microbalance illustrates the utility of these ideas in a simple structure designed for mass measurement., (© 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)