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Giant magnetostrictive thin films of double layers with gas sensitive layers as the sensing element being used to develop a gas concentration sensor were proposed in this paper. The double layers giant magnetostrictive thin films with gas sensitive layer were prepared. A magneto-mechanical coupling model was developed based on the assumption that the magnetostriction effect is equivalent to the effect of a body force. These films were tested in a cantilever arrangement and end deflection was measured. The measurement showed that the experimental results were in good agreement with the calculation results, demonstrating that the coupling model developed was effective. Furthermore, the results indicated that the giant magnetostrictive thin films with gas sensitive layer were very useful for gas concentration sensors.