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Using records of continuous seismic waveforms from 609 broadband seismic stations in the South China Block and its adjacent areas in 2010–2012, empirical Green’s functions of surface waves were obtained from cross-correlation functions of ambient noise data between these stations. High quality phase velocity dispersion curves of Rayleigh waves were obtained using time-frequency analysis. These interstation dispersion curves were then inverted to build Rayleigh wave phase velocity maps at periods of 6–50 s. The results of phase velocity maps indicate that phase velocities at 6–10 s periods are correlated with the geological features in the upper crust. Major basins and small-scale grabens and basins display slow velocity anomalies; while most of the orogenic belts and the fold belts display high velocity anomalies. With the gravity gradient zone along Taihang Mountain to Wuling Mountain as the boundary for the phase velocity maps at period of 20–30 s, the western area mainly displays low velocity anomalies, while the eastern side shows high velocity anomalies. Phase velocities in the eastern South China Block south to the Qinling-Dabie orogenic belt is higher than that in the eastern North China Block to the north, which is possibly due to the differences of tectonic mechanisms between the North China Craton and the South China Block. The phase velocities at periods of 40–50 s are possibly related to the lateral variations of the velocity structure in the lower crust and upper mantle: The low-velocity anomalies in the eastern part of the Tibetan Plateau are caused by the thick crust; while the Sichuan Basin and the southern part of the Ordos Basin display distinct high-velocity anomalies, reflecting the stable features of the lithosphere in these blocks. The lateral variation pattern of phase velocities in the southern part of the South China Block is not consistent with the surface trace of the block boundary in the eastern Yunnan Province and its vicinities. The phase velocities in the Sichuan Basin are overall slow at short periods and gradually increase with period from the central part to the edge of the basin, indicating the features of shallower basement in the center and overall stable lithospheric mantle of the basin. The middle and upper crust of the southern Ordos Basin in the North China Block is heterogeneous, while in lower crust and the uppermost mantle the phase velocities mainly exhibit high anomalies. High-velocity anomalies are widespread at the middle of the Qinling-Dabie orogenic belt, as well as the areas in southeastern Guangxi with Caledonian granite explosion, but its detailed mechanism is still unclear.