Metal-semiconductor-metal (MSM)-structured GaAs-based nanowire photodetectors have been widely reported because they are promising as an alternative for high-performance devices. Owing to the Schottky built-in electric fields in the MSM structure photodetectors, enhancements in photoresponsivity can be realized. Thus, strengthening the built-in electric field is an efficacious way to make the detection capability better. In this study, we fabricate a single GaAs nanowire MSM photodetector with superior performance by doping-adjusting the Fermi level to strengthen the built-in electric field. An outstanding responsivity of 1175 A/W is obtained. This is two orders of magnitude better than the responsivity of the undoped sample. Scanning photocurrent mappings and simulations are performed to confirm that the enhancement in responsivity is because of the increase in the hole Schottky built-in electric field, which can separate and collect the photogenerated carriers more effectively. The eloquent evidence clearly proves that doping-adjusting the Fermi level has great potential applications in high-performance GaAs nanowire photodetectors and other functional photodetectors.