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The possibility of using Fe-rich wires in mechanical stress self-sensing materials is investigated. To this end, a retrieval technique aimed to characterize the high-frequency magneto-impedance effect in ferromagnetic wires under mechanical stresses is proposed. The technique is based on the measurement of the wires inside a metallic rectangular waveguide, and it is validated through numerical simulations and tested with already published experimental data. In addition, the studied Fe-rich wires are characterized by the occurrence of the natural ferromagnetic resonance, whose frequency position increases from 7 to 8.25 GHz for elongations ranging from 0 to 60 μm.