In order to achieve high strength and toughness of the aluminum-free ultrahigh carbon steel (UHCS), the effect of a novel three-parameter combination technique including heating temperature, cooling rate, and isothermal eutectoid transformation time on the phase composition, grain morphology, and mechanical properties is investigated by X-ray diffraction analysis, optical microscopy, and mechanical tests. The result shows that when the steel is cooled from 860 8C to the eutectoid transformation temperature with the rate of 1.0 8C s À1 and held for 1.5 h, the excellent mechanical properties are obtained due to the grain refinement of carbide and matrix.