We investigated velocity and anisotropic structure of the crust beneath the eastern margin of the Tibetan Plateau to better understand its deformation and evolution mechanism. We performed H‐κ and Pms anisotropy analyses to obtain crustal thickness, Vp/Vs ratio, fast polarization direction, and splitting time from 711 stations, and further conducted quality control using slowness, harmonic and statistical analyses. The Songpan‐Ganzi Block has a large splitting time and a fast polarization direction roughly parallel to the GPS motion and SKS fast direction. It also shows an overall high but complex distribution of Vp/Vs ratio, and large variations in crustal thickness, indicating that crustal deformation is likely caused by crustal shortening and lower crustal flow. The northern Sichuan‐Yunnan Rhombic Block (SYRB) is featured by a thick crust and high Vp/Vs ratio, suggesting that the crust is likely inflated by partial melting lower crustal rocks. The subblock also exhibits a strong azimuthal anisotropy with a splitting time greater than 0.6 s. The fast polarization direction aligns with the nearly N‐S extended direction and rotates clockwise in front of the Emeishan Large Igneous Province (ELIP). The observed anisotropy agrees with aligned amphibole minerals under a simple shear condition, supporting a southward lower crust flow being diverted by the ELIP. Anisotropy measurements on the southern SYRB are less robust and widely scattered, suggesting a deformation mechanism different from the northern SYRB. In addition, the southeastern margin of the Sichuan Basin shows a systematic pattern of crustal anisotropy consistent with a pure shear deformation mechanism.