Single-crystalline cooperite (PtS) with a nearly stoichiometric composition was characterized in detail by X-ray diffraction, electron-probe X-ray microanalysis, and high-resolution scanning electron microscopy. For the first time it was demonstrated that Pt-195 static and MAS NMR spectroscopy can be used for studying natural platinum minerals. The 195pt chemical-shift tensor of cooperite was found to be consistent with the axial symmetry and is characterized by the following principal values: delta(xx) = -5920 ppm, delta(yy) = -3734 ppm, delta(zz) = +4023 ppm, and delta(iso) = -1850 ppm. According to the ESR data, the samples of cooperite contain copper(II), which is adsorbed on the surface during the layer-by-layer crystal growth and is not involved in the crystal lattice.