The invention relates to a method of sulfur removal and arsenic and mercury removal with copper smeltery tailing slurry, and belongs to the technical field of flue gas cleaning. Contaminants such as low-concentration sulfur dioxide, organic sulfur, arsenic and mercury in exhaust gas are washed out through the copper smeltery tailing slurry, wherein the organic sulfur is oxidized into sulfur-containing substances staying in the slurry; the sulfur dioxide is oxidized into sulfuric acid which can further leach out iron and zinc in tailings; arsenic trioxide is oxidized into iron arsenate precipitate; zero-valent mercury is oxidized into bivalent mercury staying in the solution; iron and zinc elements in the solid phase are leached out as the reaction goes on, such that the concentrations of iron ions and zinc ions in the solution increase continuously with the acidity of the solution strengthening and the catalytic oxidation ability gradually improving; after the completion of the reaction, the solution is placed to stand and stratify, and the sediment is collected and gathered to a cement plant to be used as raw material for cement production; and the acid leaching solution is treated to obtain iron-containing substances and metal zinc.