The tribological behaviors of nanoparticles (NPs) have attracted widespread attention in the fields of nano‐lubrication and ultra‐precision manufacturing. The frictional and dynamic behaviors of SiO2 NPs acting with the single asperity were studied on silicon surface utilizing atomic force microscope. The friction forces of NPs, both static and kinetic, exhibit an initial decrease followed by an increase as the normal load increases (0–300 nN). The nonmonotonic load‐dependence of friction behavior corresponds to the dynamic transformation of “sliding‐rolling‐sliding” motion state of the manipulated NPs, which can be predicted by a Double‐Hertz model and further confirmed by nanoindentation‐marked NPs. This research has a significant implication for regulating dynamic behaviors of NPs in contemporary three‐body abrasive tribology.