The Mechanism of Pb removal from brass scrap by compound separation using Ca and NaF addition was investigated. Because large Ca-Pb compound particles formed by Ca addition rise to the surface of the molten brass, they can be skimmed off from the molten brass. However, fine Ca-Pb compound particles remain in the molten brass because of low buoyancy. By subsequent NaF addition, the reaction between Ca-Pb compound and NaF takes place at their contact regions, resulting in the formation of solid CaF2, liquid Pb and Na gas. Pb is mainly present at the Ca-Pb compound-CaF2 interface. CaF2 acts as a binder for aggregation of fine Ca-Pb compound particles, resulting in the formation of light and large composite compounds, which rise to the surface of the molten brass. A high Pb removal rate is achieved by skimming off.