A novel core-shell particle that consists of epoxide-terminated hyperbranched polymer (HBP) and silica nanoparticles was incorporated into an epoxy/hydroxyl-terminated HBP blend to fabricate a high-performance epoxy thermoset. The effect of the core-shell particle content on the mechanical properties of the epoxy thermosets was investigated in detail. Results from tensile, flexural, and impact tests are provided. The impact fracture surface was studied by field emission-scanning electron microscopy. The incorporation of 2 wt% core-shell particles improved the tensile strength, percent elongation at break, flexural strength, and impact resistance of epoxy/hydroxyl-terminated HBP thermosets. Field emission-scanning electron micrographs showed that core-shell particle addition resulted in large-scale shear deformation and debonding from the epoxy matrix, and improved the epoxy resin toughness.