Thermoplastic vulcanizate (TPV), with both rubber‐like elasticity and plastic‐like molding processing, suggests great potential in automobile manufacturing, medical equipment, aerospace, and other fields. However, due to the poor rubber–plastic compatibility and the lack of functional elastomers, the commercial TPV is mainly prepared based on the ethylene propylene diene monomer/polypropylene (EPDM/PP) composites. Herein, we employed high vinyl polybutadiene rubber (HVBR) as the rubber phase and PP as the plastic phase to realize a novel multifunctional TPV. Benefiting from the strong rubber–plastic interfacial interaction and compatibility, the dynamically vulcanized HVBR region transformed into the island‐like phase and was uniformly distributed in the PP phases, thereby forming an even and continuous “sea‐island” structure. By optimizing the HVBR/PP blending ratio, the prepared TPV showed multifunctionality, including high mechanical strength, high elasticity, high damping, good shape memory, and repeatable processability. Collectively, the research strategy and results in this work suggest a feasible pathway toward high‐performance and multifunctional thermoplastic elastomers.