A series of polyurethane (PU)/potassium titanate whiskers (PTW) composites modified by a high molecular weight hydroxyl-terminated polydimethylsiloxane (HTPDMS) were prepared. The PTW is modified by 2,4-diisocyanatotoluene (2,4-TDI). The effect of the PTW content on the mechanical and tribological properties of the PU composites was studied. Tensile strength of the PU composites increased with the addition of PTW. The friction and wear experiments were tested on a MRH-3 model ring-on-block test rig at different sliding speeds and loads under dry sliding and water lubrication. Experimental results revealed that the small content of PTW contributed to largely improve the tribological properties of the PU composites. The coefficient of friction (COF) of the composites increased and the wear rate value decreased with increasing PTW. Scanning electron microscopic (SEM) investigations showed that the worn surfaces of the PTW-reinforced PU composites was smoother than pure polyurethane under given load and sliding speed.