The floatability of fine low-rank coal particles can be greatly influenced by their morphological characteristics, such as shape and surface roughness. In this study, the attachment efficiency and detachment amplitude of fine low-rank coal particles produced by various comminution methods onto/from the bubble surface were investigated using homemade bubble–particle wrap angle and bubble–particle attachment/detachment testing systems. Results showed that the length–diameter ratio of rod-milled products was smaller than that of crushed products. The wrap angle of particles obtained by the crushed method was larger than that obtained by the rod-milled method, i.e., particles with greater length–diameter ratio showed higher attachment efficiency onto the bubble surface. Meanwhile, particles with greater length–diameter ratio exhibited a larger detachment amplitude, which suggests that it is more difficult to be detached from the bubble surface. However, rod-milled products showed lower attachment onto the bubble surface. The flotation test confirmed that the floatability ratio of crushed products was higher than that of rod-milled products, consistent with evidence from experimental analyses. This study provides a fundamental understanding of particle shapes for low-rank coal flotation by a novel research method combining the attachment efficiency and detachment amplitude of bubble–particle combinations.