The invention discloses a composite water-treatment coagulant prepared from high-iron gibbsite and a preparation method thereof. The composite water-treatment coagulant is an aluminum chloride molten iron treatment coagulant, aluminum sulfate molten iron treatment coagulant or polyaluminum chloride molten iron treatment coagulant, which is respectively prepared from high-iron gibbsite, technical hydrochloric acid and water, or high-iron gibbsite, technical hydrochloric acid, water and calcium aluminate powder, or high-iron gibbsite, commercial sulfuric acid and water. The invention also discloses a preparation method of the composite water-treatment coagulant prepared from high-iron gibbsite. The composite water-treatment coagulant has the advantages of wide raw material sources, high iron content, high stability, wide water treatment range, favorable turbidity removal effect, simple preparation method, no need of roasting in the production process, no wastewater or waste gas emission and no environmental pollution.