For the design of stretchable and flexible high-performing materials, the reinforcement of elastomeric grades plays a crucial role. State-of-the-art fillers such as carbon black benefit from a high reinforcement but often negatively affect the processing and mixing properties of rubber compounds. To overcome this drawback, the synergistic properties of hybrid in situ filler systems are studied for EPDM compounds comprising a phenol novolac resin and ionic coagents such as zinc (meth)acrylates (ZD(M)A. With the help of a combined novolac/ZD(M)A system, the compounds could be tailored in a unique way towards higher toughness and enhanced cross-link density. Further, the fracture surface of the EPDM–novolac compounds was analyzed by scanning electron microscopy, revealing a significant change of the morphology from rough and disordered to smooth and homogenous for samples with coagents. In addition, the results clearly showed that the introduction of ionic coagents is able to compensate shares of carbon black filler in the EPDM compound. The toughening of samples with zinc (meth)acrylates is attributed to the synergistic formation of an interpenetrating polymer-filler network by simultaneous covalent and ionic cross-linking.