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This invention relates to a low-fluorine, high-calcium desulfurization slag system for electroslag remelting S-06 stainless steel and its application method, belonging to the field of electroslag special metallurgical technology. It addresses the problems of high fluorine content and pollution in existing electroslag smelting slag systems, resulting in poor uniformity of the prepared steel ingots and uneven, thick slag skin. The mass percentage of each component in the low-fluorine, high-calcium desulfurization slag system of this invention is as follows: CaF2: 38.3%~42.1%, Al2O3: 23.2%~24.8%, CaO: 30.9%~32.8%, MgO: 1.0%~5.0%, SiO2: 0.8%~1.0%, C: 0.07%~0.1%, with the remainder being impurities. The slag system of this invention exhibits good metallurgical effects; when using this slag system for electroslag remelting S-06 stainless steel, the resulting steel ingots have a uniform elemental distribution and a uniform slag skin.