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Solution-processable polyimide (PI) materials are attractive for applications in future flexible optoelectronics, owing to their excellent thermal and chemical resistance, inherent flexibility, and superior dielectric properties. They are widely integrated and investigated in various semiconductor devices. Here, the unique characteristics of PIs and their applications in optoelectronics are analyzed and summarized. A general introduction from the material aspect is given, followed by detailing the PI applications in multiple devices, including field-effect transistors, capacitors, photodetectors, and memory devices. In this review, the uniqueness and potential of PIs for next-generation optoelectronics are fully demonstrated, and the underlying challenges are proposed.