The emission of arsenic from thermal power plants poses many hazards to humans and the environment, so controlling arsenic emissions is an urgent problem to be solved. This paper prepared CuO/TiO2 adsorbent by selecting TiO2 with a large specific surface area as the substrate. The adsorption performance of CuO, TiO2, and CuO/TiO2 adsorbent materials on gas-phase arsenic at different reaction temperatures (500 °C, 600 °C, and 700 °C) was investigated. The experimental results showed that CuO/TiO2 adsorbent had better arsenic adsorption capacity than CuO and TiO2 because CuO/TiO2 has a large specific surface area and rich surface-active sites. The temperature affects the performance of the adsorbents, and all three adsorbents do not perform well at 700 °C, mainly because the metal oxide materials are not resistant to high temperatures, and the mesoporous structure is easily collapsed. CuO/TiO2 adsorbent is suitable for the control and emission reduction of heavy metal arsenic in coal-fired flue gas at medium and low temperatures below 600 °C. The above study provides a direction for developing and applying adsorbents to remove gas-phase arsenic.