Abstract: The interfacial properties of polymer/metal significantly affect the mechanical properties of composites formed by metal and polymer. Combined with thermodynamic theoretical analysis and molecular dynamics simulation, the interface fracture energy and interface strength of the interface formed by several typical polymers (Polypropylene (PP), polyethylene (PE), polystyrene (PS)) and metals (Al, Ni, Cu, Fe) were systematically calculated. With the increase of interface displacement, the interface stress of polymer/metal interface first increases, then reaches the strength and enters the interface damage stage, and the interface stress decreases until the interface is completely broken, and the stress decreases to zero. The strength change trend of different polymer/metal interfaces is consistent with the interface fracture energy, and the simulation results of interface fracture energy are basically consistent with the theoretical calculation results. The interface fracture energy of polymer/metal interface is related to the surface energy of metal. As the surface energy of metal decreases with the order of Ni, Fe, Cu and Al, the interface fracture energy of polymer/metal interface also decreases with the order of polymer/Ni, polymer/Fe, polymer/Cu and polymer/Al. Under the same metal condition, the interface strength of PE/metal and PP/metal is similar, and both are smaller than that of PS/metal. Furthermore, the interface damage was characterized by the free volume evolution of the polymer. The research results provide a basis for material selection, design and application of polymer/metal composites.