Reversible friction regulation is of long-standing great interest in the fields of both industry and scientific research, so some materials and theories have been developed aiming to solve this problem. Light-sensitive materials are promising because of the easy controllable switching of the properties and structures. Here, a reversible light-controlled macrolubrication was realized by regulating the performance of nanoscale light-sensitive molecules adsorbed on contact surfaces. In this work, symmetric diarylethene and asymmetric diarylethene had been designed and synthesized as functional materials. The friction forces were found to be obviously increased upon exposure to ultraviolet light and decayed to the initial value under visible light. In addition, the friction coefficient changed alternately with ultraviolet and visible illumination. According to the results of experiments and simulation of material properties, the behavior was suggested to be attributed to the difference in shear stiffness of the nanoscale diarylethene molecule adsorption layer triggered by two wavelength lights. This work not only provides a new lubrication regulation technology but also develops intelligent engineering materials.