Photodetectors with a broad-band response range are widely used in many fields and are regarded as pivotal components of the modern miniaturized electronics industry. However, commercial broad-band photodetectors composed of traditional bulk semiconductor materials are still limited by complex preparation techniques, high costs, and a lack of mechanical strength and flexibility, which are difficult to satisfy the increasing demand for flexible and wearable optoelectronics. Therefore, researchers have been devoted to finding new strategies to obtain flexible, stable, and high-performance broad-band photodetectors. In this work, a novel self-assembled BiGaSeAs composite superlattice-structured nanowire was developed with a simple chemical vapor deposition method for easy fabrication. After the device assembling, the photodetector showed outstanding performance in terms of obvious I on /I off (13.9), broad-band photoresponse (365−940 nm), excellent responsivity (1007.67 A/W), high detectivity (9.38 × 10 9 Jones), and rapid response (21 and 23 ms). The formation of microheterojunctions among various materials inside the nanowires also contributed to their extended broad-spectrum response and outstanding detection ability. These results indicate that the BiGaSeAs nanowires have potential applications in the field of flexible and wearable electronics.