The resonant sphere technique (RST) is applied to measurements of elastic and anelastic properties of single‐crystal periclase (MgO) in order to demonstrate the potential value of this method as an experimental technique. The lowest 22 resonant frequencies and their attenuation properties were measured in the range 1.0 to 2.6 MHz. The oscillation modes were identified by comparing the observed resonant frequencies with computed ones. Using inversion theory, we find perturbations from an assumed set of elastic constants, so that the computed frequencies agree, in a least squares sense, with the measured ones. The final values of the elastic constants were obtained by adding the perturbations to the initial values of elastic constants. Furthermore, the internal friction coefficients were determined from the observed vibrational attenuation data by a least squares method. The values of elastic constants and internal friction coefficients are in good agreement with those determined by other methods. We find better accuracy, by up to 1 order of magnitude, than that found by using the rectangular parallelepiped resonance method. The RST can be an accurate method for measuring elastic and anelastic properties of small anisotropic materials. An applicability of the RST to the Earth's free oscillation is considered. Free oscillation of an elastically anisotropic sphere shows different frequency spectrum, depending on the degree of the elastic anisotropy. The frequency spectrum of an anisotropic sphere can be interpreted as the result of the split of degenerate modes of an isotropic sphere. Therefore the anomalous splitting of the Earth's free oscillation, which cannot be explained by the rotation and ellipticity of the Earth, may be attributed to the elastic anisotropy of the Earth.