An innovative mechanical testing method (Compressive Circular Ring Method) is provided for measuring Young’s modulus of each layer in a flexible multi-layered material. The method is based on a nonlinear large deformation theory. By just measuring the vertical displacement or the horizontal displacement of the ring, Young’s modulus of each layer can be easily obtained for various thin multi-layered materials. Measurements were carried out on an electrodeposited two-layered wire. The results confirm that the new method is suitable for flexible multi-layered thin wires. In the meantime, the new method can be applied widely to measure Young’s modulus of thin layers formed by PVD, CVD, Coating, Paint, Cladding, Lamination, and others.