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Various wrinkle patterns can be formed due to the buckling of a stiff thin film on a compliant substrate. However, most wrinkled films previously reported were fixed on a large deformable substrate and thereby the potential deformability of the film was mechanically constrained by the substrate. In this study, we developed a technique for forming various wrinkled structures on the surface of a sacrificial resin layer. Since the sacrificial layer can be subsequently removed with a solvent, freestanding wrinkled films are created using the sacrificial layer. We found that a wrinkled structure is formed on the surface of the layer by applying a compressive strain to the resin layer at the appropriate moment during the hardening process. The wrinkle pattern depends on the curing time and the timing of the straining in two in-plane orthogonal directions. In addition to conventional stripe and labyrinth patterns by simple uniaxial and equi-biaxial strains, respectively, it was found that independent biaxial strains induce interesting structures, such as an orthogonally ordered wrinkle pattern and a nonsymmetrical buckling structure, in which the stripe array produced by the first straining remains and many finer wrinkles appear in each stripe by the second straining in the orthogonal direction. We conducted tensile experiments for 300-nm-thick freestanding Cu films having these wrinkled structures. The wrinkled nano-films have a variety of mechanical properties: the stripe structure has extremely high deformability (more than 10% strain) and reversibility, the labyrinth structure shows planar isotropic deformation, and the nonsymmetrical buckling structure has an anisotropic modulus and strength. Finite element analysis on the wrinkle structures revealed that the local stress concentration dominates the fracture limits.