Underwater optical communication and low-light detection are usually realized via blue-green laser sources and blue-green light-sensitive detectors. Negative-electron-affinity AlGaAs photocathode is an ideal photosensitive material for ocean exploration due to its adjustable spectrum range, long working lifetime, and easy epitaxy of materials. However, compared with other photocathodes, the main problem of AlGaAs photocathode is its low quantum efficiency. Based on Spicer’s three-step photoemission model, nanoarray structures are designed on the surface of AlGaAs photocathode to improve its quantum efficiency from two aspects of optical absorption and photoelectron transport. Through simulation, it is concluded that the cylinder with diameter of 120 nm and height of 600 nm is the best nanoarray structure, and its absorptance is always greater than 90% in the 445∼532 nm range. Moreover, the absorptance and quantum efficiency of the cylinder nanoarray AlGaAs photocathode are less affected by the incident angle. When the angle of incident light reaches 70°, the minimum absorptance and quantum efficiency are still 64.6% and 24.9%. In addition, the square or hexagonal arrangement pattern of the nanoarray has little effect on the absorptance, however, a reduction in the overall emission layer thickness will decrease the absorptance near 532 nm.