Combined studies have been conducted on the structural-phase state and physical-mechanical and tribological properties of nanostructured titanium and zirconium subjected to ion-beam implantation or microplasma oxidation. Low-temperature ion-beam nitriding of the materials examined is shown to provide a 25–35-fold increase in the wear resistance of their surface layers and a 40% decrease in the friction coefficient for tribological interaction with contact surfaces. Microplasma oxidation of titanium in aqueous solution of phosphoric acid, hydroxylapatite and calcium carbonate powders enables calcium-phosphate coatings with high physical-mechanical properties to be produced. Tribological tests in a dry friction regime and in isotonic solution of sodium chloride have revealed that a nanostructured titanium substrate-calcium phosphate coating biocomposite exhibits a fairly high friction coefficient (0.4–1.0) in tribological interactions with ultrahigh molecular-weight polyethylene or bone tissue. A substantial improvement in the tribotechnical properties of nanostructured titanium and zirconium with modified surface layers makes them very promising materials for medical and engineering applications.