Thermoplastic vulcanizates (TPVs) are multifunctional materials consisting of two or more phases with solid elastomeric properties at room temperatures and fluid-like properties above their melting point. They are produced through a reactive blending process known as dynamic vulcanization. The most widely produced TPV type is ethylene propylene diene monomer/polypropylene (EPDM/PP), which is the focus of this study. The peroxides are mainly selected to be used in crosslinking of EPDM/PP-based TPV. However, they still have some disadvantages, such as the side reactions resulting in the beta chain scission of the PP phase and undesired disproportionation reactions. To eliminate these disadvantages, coagents are used. In this study, for the first time, the use of vinyl functionalized polyhedral oligomeric silsesquioxane (OV-POSS) nanoparticles was investigated as a potential coagent in EPDM/PP-based TPV production via peroxide-initiated dynamic vulcanization. The properties of the TPVs having POSS were compared with the conventional TPVs containing conventional coagents, such as triallyl cyanurate (TAC). POSS content and EPDM/PP ratio were investigated as the material parameters. Mechanical properties of EPDM/PP TPVs exhibited higher values in the presence of OV-POSS, which resulted from the active participation of OV-POSS into the three-dimensional network structure of EPDM/PP during dynamic vulcanization.