<p>Few studies have investigated the influence of hydrophobic graphite (anode materials) on the entrainment behavior of hydrophilic lithium metal oxides (cathode materials, LMOs) during froth flotation of spent lithium-ion batteries (LIBs), despite their coexistence in the flotation pulp. This paper conducted experimental studies on the entrainment behavior of lithium nickel cobalt manganese oxide (NCM) in the absence and presence of spheroidized graphite and explained the worse flotation efficiency of spheroidized graphite in the presence of NCM. Particle size distribution tests, contact angle measurements and froth flotation tests were conducted on battery-grade graphite and NCM mineral. The results demonstrated that pure spheroidized graphite readily floated, whereas pure fine NCM particles were easily entrained into the flotation concentrate. The flotation test results of the artificial mixture of battery-grade NCM and graphite indicated that the solid concentration and hydrophobic graphite had significant impacts on NCM entrainment. The addition of hydrophobic graphite greatly reduced the entrainment of NCM, but the entrainment degree of NCM continued to increase as the graphite content increased. The effect of NCM on the flotation efficiency of spheroidized graphite showed that the entrainment or entrapment of NCM decreased the flotation efficiency of spheroidized graphite. The study provides significant new insights into black mass flotation separation, building a foundation for further improvements in the separation of black mass from spent LIBs.</p>