Epoxy resin is an of the most widely used adhesives for various applications owing to its outstanding properties. The performance of epoxy systems varies significantly depending on the composition of the base resin and curing agent. However, there are limitations in exploring numerous formulations of epoxy resins to optimize adhesive properties because of the expense and time-consuming nature of the trial-and-error process. Herein, molecular dynamics (MD) simulations and machine learning (ML) methods were used to overcome these challenges and predict the adhesive properties of epoxy resin. Datasets for diverse epoxy adhesive formulations were constructed by considering the degree of crosslinking, density, free volume, cohesive energy density, modulus, and glass transition temperature. A linear correlation analysis demonstrated that the content of the curing agents, especially dicyandiamide (DICY), had the greatest correlation with the cohesive energy density. Moreover, the content of tetraglycidyl methylene dianiline (TGMDA) had the highest correlation with the modulus, and the content of diglycidyl ether of bisphenol A (DGEBA) had the highest correlation with the glass transition temperature. An optimized artificial neural network (ANN) model was constructed using test sets divided from MD datasets through error and linear regression analyses. The root mean square error (RMSE) and correlation coefficient (R²) showed the potential of each model in predicting epoxy properties, with high linear correlations (0.835–0.986). This technique can be extended for optimizing the composition of other epoxy resin systems.