Surface roughness of particles plays an important role in bubble-particle interaction process. However, the continuous attachment and detachment process have rarely been characterized between the surface of different roughness and air bubble. In this study, the continuous attachment and detachment processes between the surface of different roughness and air bubble were investigated by a highly sensitive microbalance. The bubble–surface interaction process was monitored by a high-speed camera to analyze the geometry parameters, including distance, adhesion diameter, and contact angle. It was found that the bubble-particle attachment time increased with the increase of surface roughness. The magnitude of the repulsive force in the bubble-surface approaching process increased with the increase of surface roughness, while the attractive force in the bubble-particle retracting process decreased monotonically with the surface roughness. The force measured by microbalance was finally compared with the calculated one. The calculated force at the biggest force point also increased with the decrease of surface roughness. These results indicate that coal particles with lower surface roughness, which have less water-filled pores and pillars, is more conducive to flotation due to the lower repulsive force in the bubble-particle attachment process and higher adhesive force in the bubble-particle detachment process, and vice versa.