In this review, the primary focus is the recent advances in the development of freestanding inorganic crystalline semiconductors and their manipulation technology for flexible optoelectronic applications. We firstly cover the details of the growth and processing techniques of freestanding inorganic crystalline semiconductors in various dimensions and their material property under strain condition. Finally, fabrication processes and opto-electrical properties of flexible optoelectronics are introduced. Future research directions are also discussed, including further enhancement of device performance, building more types of optoelectronic devices on flexible substrates, and process integration for the advanced optoelectronic circuits and systems.