The insufficient lubrication of the contact interface between moving parts can easily induce severe friction vibration and noise under extreme working conditions, which will threaten the service life and reliability of polymer moving components, including water-lubricated stern tube polymer bearings. Thermoplastic polyurethane (TPU) modified by polytetrafluoroethylene (PTFE) particles was developed. The effects of PTFE on the wear and vibration behaviors of modified TPU sliding against the ZCuSn10Zn2 ring-plates were investigated. The coefficients of friction (COFs), wear mass losses, wear morphologies, frictional vibration, and noise were analyzed synthetically. The results showed that a suitable mass content of PTFE reduced the COFs and wear mass losses of the TPU composites by more than 50% and 40%, respectively, while presenting an excellent friction reduction. The lower COFs of modified TPU showed a small fluctuation amplitude and eliminated vibration waveforms at high vibrational frequencies, which was useful for reducing frictional vibration and noise. The knowledge gained in this study is useful for a better understanding of the wear behaviors of polymer composites, as well as for the design a new polymer material with good self-lubricating and frictional vibration and noise reduction properties.