Interactions occurring at the polymer and mold interface during injection molding significantly affect inherent filling behavior and cavity replication quality. The chemistry of the contact between the polymer and mold is important when considering the heat transfer occurring at the interface, macromolecular adsorption at the mold surface, and the overall ability of the polymer to replicate the mold surface. In this work, we study the correlation between surface energy and polymer contact angle for coated injection molds, aiming at further the understanding of polymer/mold interface interactions. Different surface coatings are deposited on sample steel surfaces to modify the surface energy and affect the chemistry of the polymer/mold contact. The surface energy of these differently coated steel surfaces is characterized by measuring contact angle with two different liquids (water and diiodomethane), and by using the Fowkes method. The wetting behavior of different thermoplastic resins is evaluated by monitoring their contact angle at the melt temperature over the coated surfaces. The physical modeling of the interface properties is then correlated to injection molding experiments. The effect of coatings on polymer/mold interface tribology is studied by considering surface quality, cavity pressure distribution, and surface energy of the molded plastic parts.