Flotation tests with intergrown particle liberation were conducted to explore a separation method of difficult-to-separate coking coal from the Tangshan Kailuan mine in China. The particle size distribution, density and coal petrography were investigated. The difficult-to-separate coking coal sample resulted in intergrown particles, such as non-liberated coal and rocks. Thus, intergrown coal particle liberation and re-separation tests were conducted. The results showed that grinding time had a great effect on the flotation performance. Grinding prompted coal to dissociate and improve the surface hydrophobic properties of minerals. However, heterogeneous fine silt covered the surface of coal particles when coal was ground too long. The inorganic mineral particles were over-ground and reduced the contact angle of coal. The results of coal rock dissociation and laboratory re-separation tests showed that clean coal combustible recovery increased through intergrown particle liberation and re-separation.