Single‐crystalline silicon (sc‐Si) is the dominant semiconductor material for the modern electronics industry. Despite their excellent photoelectric and electronic properties, the rigidity, brittleness, and nontransparency of commonly used silicon wafers limit their application in transparent flexible optoelectronics. In this study, a new type of Si microstructure, named single‐crystalline Si frameworks (sc‐SiFs), is developed, through a combination of wet‐etching and microfabrication technologies. The sc‐SiFs are self‐supported, flexible, lightweight, tailorable, and highly transparent. They can withstand a small bending radius of less than 0.5 mm and have a transparency of up to 96% in all wavelength ranges, owing to the hollowed‐out framework structures. Thus, the sc‐SiFs provide a new platform for high‐performance transparent flexible optoelectronics. Taking transparent flexible photodetectors (TFPDs) as an example, substrate‐free and self‐driven TFPDs are achieved based on the sc‐SiFs. The devices exhibit superior performance compared to other reported TFPDs and reveal the great potential for integrated optoelectronic applications. The development of sc‐SiFs paves the way toward the fabrication of high‐performance transparent flexible devices for a host of applications, including e‐skins, the Internet of Things, transparent flexible displays, and artificial visual cortexes.