A plasma-enhanced atomic layer deposition (PE-ALD) system was used to deposit magnesium zinc oxide (MgxZn1−xO) films with various Mg content (x). The MgxZn1-xO films were applied to metal–semiconductor–metal ultraviolet (UV) photodetectors (MSM-UPDs) as an active layer. The Mg content in the MgxZn1-xO films was modulated by adjusting the ZnO–MgO cycle ratios to 15:1, 12:1, and 9:1. Correspondingly, the Mg content in the MgxZn1-xO films characterized using an energy dispersive spectrometer was 0.10, 0.13, and 0.16, respectively. The optical bandgap of the MgxZn1-xO films increased from 3.56 to 3.66 eV with an increase in Mg content from 0.10 to 0.16. The peak position of photoresponsivity for the MgxZn1-xO MSM-UPDs was also shifted from 350 to 340 nm. The UV-visible rejection ratios of the MgxZn1-xO MSM-UPDs were higher than 3 orders of magnitude. In addition, excellent detectivity and noise equivalent power for the MgxZn1-xO MSM-UPDs were observed at a bias voltage of 5 V. The high performance of the MgxZn1-xO MSM-UPDs was achieved by PE-ALD at a low temperature.

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