Dynamically vulcanized poly(vinyl chloride)-epoxidized natural-rubber thermoplastic elastomers (PVC-ENR TPEs) were prepared using a semi-EV vulcanization system. The compounds were melt-mixed, and the rheological behavior was evaluated. The effect of curatives concentration on the theological behavior using the shear dependence of viscosity and the activation energy for viscous flow was evaluated. Viscoelastic behavior was also investigated with the Monsanto MDR 2000. The parameters studied include the elastic modulus at maximum torque, the loss peak at maximum torque, and their ratio (tan delta). The data obtained were correlated with the material properties, such as hardness and resilience.