The bio-based thermoplastic vulcanizates (TPVs) composed of polylactic acid (PLA) and epoxidized natural rubber (ENR) was prepared by the dynamic vulcanization method induced by dicumyl peroxide (DCP), and a novel filler, bis(aminopropyl)-terminated polydimethylsiloxane (PDMS-NH 2 ), was added as the compatibilizer. The dynamic vulcanization reaction occurred first, and the PLA-g-ENR graft copolymer was formed at the interface of PLA and ENR.With the addition of appropriate amount of PDMS-NH 2 , the cross-linking of ENR was enhanced, and the size of PLA became smaller and more evenly dispersed. The prepared TPVs were found to have dual interfacial compatibilization networks. Mechanical characterization of this polymeric material containing a special structure is performed. TPV achieved the tensile strength at break of 12.8 MPa and elongation at break of 103%, revealing 103% and 329% higher than 6.3 MPa and 24% for the simple blend of ENR/PLA. Meanwhile, the elastic modulus of TPV increased to 352 MPa, which was 1.96 times that of the simple blend. As a result, ENR/PLA composites with high toughness and mechanical strength are achieved and the toughening mechanism and toughening factors were discussed.