Abstract Active control of nanotribological properties is a challenge. Materials responsive to external stimuli may catalyze this paradigm shift. Recently, the nanofriction of a thin film is modulated by light, ushering in phototribology. This frontier is expanded here, by investigating photoactive nanoparticles in lubricants to confer similar functionality to passive surfaces. Quartz‐crystal microbalance (QCM) is employed to assess the phototribological behavior of aqueous suspensions of titanium dioxide nanoparticles. A comparison of dark and illuminated conditions provides the first demonstration of tuning the interfacial friction in solid‐nanosuspension interfaces by light. Cyclic tests reveal reversible transitions between higher (dark) and lower friction (illuminated) regimes. These transitions are underpinned by transient states with surface charge variations, as confirmed by Zeta potential measurements. The accumulated surface charge increases repulsion within the system and favors sliding. Upon cessation of illumination, the system returns to its prior equilibrium state. These findings impact not only nanotribology but nanofluidics and nanorheology. Furthermore, the results underscore the need to consider light‐induced effects in other scenarios, including the calculation of activity coefficients of photoactive suspensions. This multifaceted study introduces a new dimension to in operando frictional tuning, beckoning a myriad of applications and fundamental insights at the nanoscale.