The invention discloses a method for removing arsenic and recovering valuable metal from ilmenite smoke dust. The method comprises the steps of leaching ilmenite smoke dust through strong alkali to obtain a leaching solution containing arsenate and zincate and iron-containing leaching slag; adding benzyl chloride to the leaching solution to convert arsenate into benzyl-arsine; then adding a particle carrier for adsorbing the benzyl-arsine; fully floating and separating to obtain benzyl-arsine salt; neutralizing the floating separating liquid core, and separating out a zinc hydroxide product; adding water to the iron-containing leaching slag; stirring and mixing the slurry; and then adding a flocculating agent and a collecting agent for floating and separating so as to obtain iron ore concentrate. With the adoption of the method, the purpose of removing arsenic is achieved, and moreover, iron and zinc products can be recovered, so that the resource comprehensive utilization of the ilmenite smoke dust can be realized; and the method is simple, quick, efficient, and low in cost and meets the industrial production.