Improving running-in quality is an important project of Green Tribology. In actual environment, the running-in quality of mechanical equipment is greatly affected by system parameters. In view of this, running-in experiments were performed at different rotating speeds on a pin-on-disc tribometer. Chaos theory was used to investigate the effect of rotating speeds on the running-in quality. The experimental results showed that the running-in quality could be better evaluated by using the chaotic characteristic parameter “Convergence (CON)”. The greater the CON, the better the running-in quality. With an increase of the rotating speed, CON first gradually increased and then decreased to a certain level, whilst the running-in quality first gradually became better and then became worse. A moderate rotating speed is advantageous to obtain the optimum running-in quality. This contributes to the service life extension and the efficiency improvement, so as to reduce energy consumption.