Thermoplastic vulcanizates (TPVs) are among the most concerned polymer materials because they exhibit a combination of good elasticity and easy processibility and recyclability. Herein, a beta-nucleating agent (beta-NA) was introduced into ethylene propylene diene monomer (EPDM)/polypropylene (PP) TPVs through a simple and effective postprocessing method to induce the formation of beta-PP crystals for preparing highperformance TPV products. High content of beta-PP crystals is achieved in TPV, but the total crystallinity of the PP matrix remains constant. Unexpectedly, both mechanical strength and elasticity of TPV with beta-PP crystals (beta-TPV) are significantly higher than those of TPV with a-PP crystals (alpha-TPV). The change in the structure of both alpha-TPV and beta-TPV during real-time deformation and the deformation mechanism was carefully studied by combining Synchrotron two-dimensional wide-angle X-ray diffraction (2D-WAXD) and atomic force microscopy nanomechanical mapping (AFM-NM) techniques. The mechanism for the simultaneous improvement of mechanical strength and elasticity of TPV is revealed.