We first report on the Love wave tomography of China based on ambient noise cross-correlations. We used 3 years of continuous waveform data recorded by 206 broadband seismic stations on the Chinese Mainland and 36 neighboring global stations and obtained Love wave empirical Green’s functions from cross-correlations of the horizontal components. The Love wave group velocity dispersion measurements were used to construct dispersion maps of 8- to 40-s periods, which were then inverted to obtain a three-dimensional horizontally polarized S-wave (SH) velocity structure. The resolution was approximately 4° × 4° and 8° × 8° for eastern and western China, respectively, and extended to a depth of approximately 50 km. The SH model was generally consistent with a previously published vertically polarized S-wave (SV) model and showed large-scale features that were consistent with geological units, such as the major basins and changes in the crustal thickness across the north-south gravity lineament. The SH and SV models also showed substantial differences, which were used to examine the subsurface radial anisotropy. We define the radial anisotropy parameter as . At a shallow depth, we observed significant radial anisotropy under major basins, which may be related to thick sedimentary layers. At the mid to lower crust, most of the Chinese continent showed strong positive radial anisotropy (SH > SV). Central and southern Tibet showed strong positive anisotropy, whereas the radial anisotropy was relatively weak at the northern and eastern margins, which suggests a change in deformation style from the plateau interior to its margins. The North China craton showed prominent positive radial anisotropy, which may be related to decratonization and strong extension since the Mesozoic Era. Love waves are less well retrieved than Rayleigh waves from ambient noise cross-correlations. Increasing the duration of the cross-correlation data beyond 4 to 8 years may not aid in retrieving Love waves of longer periods, for which improved methods need to be explored.