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The recent efforts in exploiting semiconductor nanowires (NWs) for high-performance macroelectronics are reviewed. In brief, a new concept of NW thin-film transistors (NW-TFTs) has been proposed and demonstrated from oriented semiconductor NW thin films. In NW-TFTs, the source and drain electrodes are bridged by multiple single-crystal NWs in parallel. Therefore, charges travel from source to drain within single crystals, ensuring high carrier mobility. Recent studies have shown that high-performance NW-TFTs and high-frequency circuits can be produced from silicon NWs on a variety of substrates, including glass and plastics, using a solution assembly process. The device performance of these NW-TFTs not only greatly surpasses that of solution-processed organic TFTs but is also significantly better than that of conventional amorphous or polycrystalline silicon TFTs, approaching single-crystal silicon-based devices. Furthermore, with a similar framework, group III-V or II-VI NW or nanoribbon materials of high intrinsic carrier mobility or optical functionality can be assembled into thin films on flexible substrates to enable new multifunctional electronics/optoelectronics that are not possible with traditional macroelectronics. This approach thus opens a new avenue to high-performance flexible macroelectronics and will not only impact existing applications but also enable a whole new generation of flexible, wearable, or disposable electronics for computing, storage, and wireless communication.