Monolayer Ta and multilayer Ti/Zr/Ta and Zr/Ti/Ta coatings were prepared by magnetron sputtering on TC4 substrates to improve the surface friction and wear properties in a simulated body fluid (SBF) environment and an atmospheric environment. Optical microscopy, scanning electron microscopy, laser scanning confocal microscopy and nano scratch testing were employed to establish the structure-property-environment relationships. By controlling the preparation parameters, the outermost layer of all three samples was Ta coating, and the total coating thickness of each sample was about 3 μm. Friction and wear testing revealed that, compared to bare TC4 substrate, and multilayer Ti/Zr/Ta and Zr/Ti/Ta coatings, the monolayer Ta possessed the lowest friction coefficient as well as the minimum wear rate (i.e., calculation result of the wear track width and wear depth). This was mainly attributed to excellent adhesion strength, a particular structure and solid lubrication of the monolayer coating. The same coating sample exhibited a stronger wear resistance in the SBF environment than in the atmospheric environment. Furthermore, the wear behaviors and mechanisms of various coatings under different experimental environments are also discussed.