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In this study examining the effects of temperature and dissolved oxygen (DO) on arsenic (As) release at the sediment–water interface (SWI), it was found that an increase in temperature promoted the formation of an anaerobic environment and the reduction and desorption of As fractions within the sediments. A temperature of 32 °C was the most favorable condition for As release at the SWI, and low DO conditions aggravated this process. Even under high DO conditions, the release of sediment As was significantly accelerated under high-temperature conditions, allowing dissolved As to rapidly migrate to the overlying water. In this process, the release of As from sediments was a consequence of the transformation of As fractions in the sediments.