The interfacial fracture performance of dicyandiamide cured epoxy/steel adhesive systems was thoroughly investigated. Fracture mechanics based testing was utilized to study several variables which were believed to influence the epoxy/steel interphase region, specifically the elasomeric toughener concentration, the dicyandiamide concentration, and the cure temperature. Bulk mechanical measurements were conducted to provide background information for comparison with the fracture data, and surface analyses were carried out on the neat adhesives and failed fracture specimens to provide insight into the locus and causes of failure. The addition of toughener drastically impacted the morphological, bulk mechanical, and adhesive properties in these latent cure systems. Modulus values decreased and bulk fracture toughness values increased with increasing toughener content. Static double cantilever beam (DCB), fatigue DCB, and notched coating adhesion (NCA) interfacial fracture performances all increased. X-ray photoelectron spectroscopy (XPS) and tunneling electron microscopy (TEM) analyses of the failed specimens revealed that chemical changes were more prominent at the epoxy/steel interphase than in the bulk of the materials. Morphological variations were also apparent with toughener level variations, but for a single formulation no differences between the bulk and intephase morphologies were seen. Evaluations were conducted on a series of elastomer modified model epoxy formulations cured with varying amounts of dicyandiamide. The modulus and bulk fracture toughness values were shown to be independent of dicyandiamide concentration, whereas the adhesive performance was greatly influenced. For increases in the concentration of dicyandiamide, single lap shear (SLS) failure strength values increased while quasi-static DCB and NCA test performances decreased. Fatigue DCB results showed improved adhesive performance at both high and low levels of dicyandiamide content. The results of the failure surface evaluations suggest that dicyandiamide variations produce significant chemical changes only in the epoxy/steel interphase region, and not in the bulk. Analyses were conducted on all of the above systems using two additional cure temperatures. The purpose of this work was to alter the dicyandiamide solubility, and possibly the dicy/epoxy reaction mechanisms, and to determine what influence these changes had on the interfacial fracture performance. In general it was found that performance increased as the cure temperature was increased. / Ph. D.