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In the present study, a processing technique for recycling investment casting ceramic shell waste was proposed to separate valuable refractory aggregate zircon sand. The microstructure and phase constituents of the shell waste and separation process were investigated. The results show that the characteristics of microstructure and phase constituents of the shell waste can meet the conditions for preferentially separating zircon sand, and zircon sand can be separated by gravity separation on a shaking table. The separated zircon sand has good shape and high purity, and can be used for the production of castings and other applications.