The structure of biocompatible titanium alloys and coatings, nanostructured by rapid plastic deformation technology, thermomechanical treatment, and magnetron sputtering, is studied. Measured indentation is used to obtain a mechanical property database. Values of hardness, elasticity modulus, and elastic recovery of titanium, and also Ti–Ni alloys with shape memory and a superelasticity effect Ti–Nb–Zr, Ti–Nb–Ta that are in microstructured and nanostructured conditions, are measured. It is shown that with indentation of a Vickers diamond indenter into a TiCCaPCON coating deformation proceeds inhomogeneously by periodic formation of shear steps.