The invention relates to a method for removing iron and fluorine through a synergistic leaching solution of leaching residues in high iron-bearing zinc calcine and high iron-bearing zinc sulfide concentrate. The method comprises the following steps: pumping the synergistic leaching solution of leaching residues in high iron-bearing zinc calcine and high iron-bearing zinc sulfide concentrate into a pressure kettle by a pressure pump, adding ferric oxide crystal seeds, leading in industrial oxygen or oxygen-enriched air, controlling the partial pressure of the led-in gas, in-kettle total pressure and temperature, reacting under the stirring condition so as to enable ferrous ions in the solution to be in the oxidization hydrolysis reaction under the hydrothermal condition to form ferric oxide crystals with a certain specific surface area, wherein the ferric oxide crystal has a strong adsorption action on fluorine ions in the solution. The high-efficiency oxidization hydrolysis of ferrous ions and purification and fluorine removal can be realized under the oxygen pressure and hydrothermal conditions, the ferrum removal rate in the whole process is higher, the adsorption quantity of the ferric oxide crystals on fluorine is higher, the concentration of liquid iron ions is lower after the iron and fluorine are removed, the iron-bearing high-grade ferrum oxide residues with stable properties can be obtained, and has hidden application values in forming iron and steel industry raw materials or cement additives.