The ability to create and manipulate large arrays of inorganic semiconductor micro/nanostructures for integration on unconventional substrates provides new possibilities in device engineering. Here, simple methods are described for the preparation of structures of single crystalline silicon in suspended and tethered configurations that facilitate their deterministic assembly using transfer-printing techniques. Diverse shapes (e.g., straight or curved edges), thicknesses (between 55 nm and 3 μm), and sizes (areas of 4000 μm2 to 117 mm2) of structures in varied layouts (regular or irregular arrays, with dense or sparse coverages) can be achieved, using either flat or cylindrical roller-type stamps. To demonstrate the technique, printing with 100% yield onto curved, rigid supports of glass and ceramics and onto thin sheets of plastic is shown. The fabrication of a printed array of silicon p+–i–n+ junction photodiodes on plastic is representative of device-printing capabilities.