Frequency‐selective surfaces (FSS) with flexible treatment can be employed in various applications. This paper develops a mechanically constructed flexible double‐layer adjustable FSS based on a 3D cross‐shaped kirigami structure design. Through mechanical stretching, the kirigami structure partly adhered to the ecoflex substrate enables this FSS to modulate the resonant frequencies of two filter bands synchronously. Meanwhile, the structural deformation triggered by mechanical stretching may function as a switch to adjust the filter band with a higher resonant frequency. According to the results of EM experiments and simulations, in the absence of stretching, the undeformed FSS with a double‐layer structure has two filter bands. Compared to the undeformed configuration, the stretching induces structural deformation, which results in apparent resonant frequency shifts of both the two filter bands and the contraction of the filter band with higher resonant frequency. A buckling model that has been theoretically, cumulatively, and experimentally proven is utilized to investigate the structural deformation of this FSS caused by stretching. It is convenient to switch flexible double‐layer adjustable FSS' deformation by mechanical method. This flexible double‐layer adjustable FSS offers a new design strategy for the application of FSS, paving the route for new developments in electromagnetic compatibility.