Tellurium nanowires (NWs) are attractive one-dimensional materials for many applications, yet most synthesis processes require hazardous chemical reducing agents and extreme operating conditions. Here we described a solvothermal synthesis of Te NWs using a non-toxic reducing agent, ascorbic acid. Then the Te NWs were assembled into a well-aligned film through a stirring-assisted oil-water-air interface assembly method and a Te NWs photodetector was fabricated which is sensitive to infrared radiation. The photodetector based on the well-aligned Te NWs film had a series of more excellent photoelectric properties than that based on those being randomly oriented. For example, the photoresponsivity of the former is 103 times larger, and the response time is 1.15 × 103 times shorter, than those of the latter.