The separation of graphite from cathode active materials containing Co, Ni, and Mn, and the metals Cu and Al by flotation was tested and evaluated with a black mass sample of crushed spent Li-ion batteries. The metals, Cu and Al, were mostly (>90%) concentrated by sieving into an oversize fraction (+0.25 mm). Graphite and the cathode active materials in the oversize fraction (+0.25 mm) were effectively separated from the metals, Cu and Al, by flotation. Pre-treatment by roasting at a temperature of 350–450 °C improved the flotation efficiency of graphite from the cathode active materials for the undersize fraction (−0.25 mm).