Complex, three dimensional (3D) assemblies of nanomaterials provide sophisticated, essential functions in even the most basic forms of life. Compelling opportunities exist for analogous 3D structures in man-madedevices, but existing design options are highly constrained by comparatively primitive capabilities in fabrication and growth. A recent collection of advanced concepts in thin film physics, materials science and mechanical engineering provide broad access to diverse, highly engineered classes of 3D architectures in diverse classes of functional materials and devices, with characteristic dimensions that range from nanometers to centimeters and over areas that span square centimeters or more. The approach relies on geometric transformation of preformed two dimensional (2D) precursor micro/nanostructures and/or devicesinto extended 3D layouts by controlled processes of substrate-induced compressive buckling, where the bonding configurations, thickness distributions and other parameters control the final configurations. This talk reviews the key concepts, and focuses on the most recent developments with several example applications at the bio-interface.