An approach based on film buckling under simple uniaxial tensile testing was utilized in this paper to quantitatively estimate the interfacial energy of the nanostructured multilayer films (NMFs) adherent to flexible substrates. The interfacial energies of polyimide-supported NMFs are determined to be *5.0 J/m 2 for Cu/Cr, *4.1 J/m 2 for Cu/Ta, *2.8 J/m 2 for Cu/Mo, *1.1 J/m 2 for Cu/Nb, and *1.2 J/m 2 for Cu/Zr NMFs. Furthermore, a linear relationship between the adhesion energy and the interfacial shear strength is clearly demonstrated for the Cu-based NMFs, which is highly indicative of the applicability and reliability of the modified models.