Despite that the negative effects of lizardite on pentlandite flotation have been realized, the lizardite effects under different slurry pH have not been sufficiently investigated. Micro-flotation test results showed that pentlandite recovery gradually decreased with the increase in slurry pH when lizardite slime existed. Both electro-kinetic tests and turbidity measurements indicated that hetero-coagulation between the pentlandite and lizardite particles occurred in the entire pH range, which failed to explain the lower recovery at high slurry pH. Zeta potential distribution measurements and sedimentation tests suggested that self-coagulation among lizardite particles occurred at higher pH, which increased the amount of lizardite slime coated on the pentlandite surfaces and thus reducing collector adsorption and flotation recovery. The particle interaction in the pentlandite/lizardite flotation system was investigated using DLVO theory and microscope observation. The findings of the study will contribute to the improvement in pentlandite flotation by regulating the particle interactions.