The tribo-dynamic behaviors of third-body colloidal particles (CPs) at the soft–hard contact interface significantly impact the substrate surface performance. To explore the differences of the stick-slide and roll-slide tribo-dynamic behaviors of CPs, the tribological behaviors of fixed and free CPs on hydrophilic silicon substrates were investigated using the colloid probe and nano-manipulation technology in atomic force microscopy, respectively. In contrast to the velocity-enhanced static friction commonly observed in fixed CPs, the static friction of free CPs exhibits a logarithmic decrease with increasing velocity. This phenomenon can be attributed to the transition from a “sliding-dominated” to a “rolling-dominated” driving state of the CPs as velocity increases. The findings enhance the understanding of tribo-dynamic behaviors of CPs at the nanoscale and provide a foundation for the deliberate design and optimization of CP-based applications in chemical mechanical polishing (CMP) and post-CMP cleaning technologies.