AbstractEpoxy film adhesives are typically used in different industries. However, these adhesives suffer from brittleness, low flexibility, and thermal stability problems. In this research, phenolic resin (Novolac) and poly (butyl acrylate‐block‐styrene) were used in the formulation of epoxy film adhesive (Diglycidyl ether bisphenol A) to increase thermal stability and adhesion strength and as the toughening agent, respectively. Alumina nanoparticles were also employed to enhance the mechanical properties. The influence of block copolymer and alumina nano particles was also assessed on the mechanical and thermal properties of epoxy‐based film adhesives. The investigation of the mechanical properties of dumbbell‐shaped samples and adhesion strength of the Al‐Al bonded joints were evaluated by tensile, lap shear, and T‐peel tests. The thermal stability of the optimal samples was assessed by thermogravimetry analysis (TGA). SEM analysis was also utilized to study the toughening mechanism. Tensile test of the dumbbell‐shaped samples indicated that the incorporation of 2.5 phr block copolymer and 2 phr alumina nanoparticles enhanced the toughness to 250%. The shear and peel strengths of this sample also exhibited 51% and 76% increase, respectively, showing a remarkable synergistic effect. On the other hand, TGA results revealed that the incorporation of block copolymer improved the thermal stability of the adhesive matrix. The copresence of these two materials also showed a considerable synergistic effect on the thermal stability. The SEM results were also in line with the results of mechanical tests as the crack deviation, crack pinning, and debonding were the most important mechanisms of toughening.Highlights A new platform was developed for designing epoxy films adhesives with high mechanical, adhesion, and thermal properties. The hybrid of butyl acrylate block styrene copolymer, phenolic resin, and alumina nanoparticles showed synergistic effects on the lap shear and T‐peel strength. The greatest improvement in toughness was related to the epoxy adhesive containing 2.5 phr block copolymer and 2 phr alumina nanoparticles. Analysis of the fracture surface showed that by using hybrid of nanoparticles and block copolymers in the epoxy film adhesive formulation, the cohesive failure occurred. The use of hybrid additives in film adhesive formulations enlightened manufacture of adhesives for future studies on adhesive formulations.