This paper describes the application of Taguchi experimental design to a nano-structure film. An L9 orthogonal array and a molecular dynamics simulation were used to design a metal film made up of eight atomic layers so that the metal film was made to have strong adhesion to a wholly aromatic polyester resin. By carrying out sensitivity analysis with the orthogonal array, among four metal-film factors (the short-side and long-side lattice mismatches with the resin Δa and Δb, surface energy G, and cohesive energy H of an atomic-layer laminated metal film), the mismatches were found to be the most dominant factors in the adhesion strength. The author also found that reducing the mismatches and increasing the surface energy and cohesive energy are effective in increasing the adhesion strength and the signal-to-noise ratio. Molecular simulations showed that a copper/ruthenium/cobalt-laminated film is an appropriate structure that has strong adhesion to the polyester resin.