Tribological behavior of biomedical ultrafine-grained (UFGed) TiNbZrTaFe (TNZTF) composites fabricated by powder metallurgy was investigated under dry wear condition. Results show that compared with two kinds of conventional biomedical Ti–6Al–4V (TAV) and Ti–13Nb–13Zr (TNZ) alloys, the wear loss of the TNZTF samples is only 3.5% and 1% of that of the TAV and TNZ samples, respectively. Unusual tribological behavior is that the wear loss of the TNZTF samples decreases with the increase in sliding speed at the same load. This is attributed to the formation of a large amount of hard Nb2O5 particles on the contact surface of the material during rubbing and more severe plastic deformation in the material layers adjacent to the contact surfaces. The wear mechanism of the three kinds of alloys was also investigated. The outstanding tribological property proves that the UFGed TNZTF alloys should be an excellent candidate material to be used for biomedical application in the future.