Proof-of-concept, first metal-semiconductor-metal ultraviolet photodetectors based on nanocrystalline gallium nitride (GaN) layers grown by low-temperature hollow-cathode plasma-assisted atomic layer deposition are demonstrated. Electrical and optical characteristics of the fabricated devices are investigated. Dark current values as low as 14 pA at a 30 V reverse bias are obtained. Fabricated devices exhibit a 15× UV/VIS rejection ratio based on photoresponsivity values at 200 nm (UV) and 390 nm (VIS) wavelengths. These devices can offer a promising alternative for flexible optoelectronics and the complementary metal oxide semiconductor integration of such devices.