We report high-performance photodetectors of individual single crystalline Zn3P2 nanowires. A facile catalyst-free physical evaporation process was developed to synthesize high-quality single crystalline Zn3P2 nanowires (NWs) with high yield. A typical individual Zn3P2 NW photodetector exhibited fast speeds (the response and recovery times were less than 25 and 26 μs, respectively) and high gain (∼470), which is an excellent result towards getting a balance in the speed and gain trade-off of the semiconductor nanostructure-based photodetectors. In addition, the device had the advantages of high photosensitivity (Iphoto − Idark/Idark ≈ 100) and small device size (constructed on an individual nanowire). All these merits substantiate that the Zn3P2 nanowires can serve as excellent photoconductive materials, and the Zn3P2 NW photodetectors are very promising for practical applications.