Due to their superior mechanical properties, 2D materials have gained interest as active layers in flexible devices co‐integrating electronic, photonic, and straintronic functions altogether. To this end, 2D bendable membranes compatible with the technological process standards and endowed with large‐scale uniformity are highly desired. Here, it is reported on the realization of bendable membranes based on silicene layers (the 2D form of silicon) by means of a process in which the layers are fully detached from the native substrate and transferred onto arbitrary flexible substrates. The application of macroscopic mechanical deformations induces a strain‐responsive behavior in the Raman spectrum of silicene. It is also shown that the membranes under elastic tension relaxation are prone to form microscale wrinkles displaying a local generation of strain in the silicene layer consistent with that observed under macroscopic mechanical deformation. Optothermal Raman spectroscopy measurements reveal a curvature‐dependent heat dispersion in silicene wrinkles. Finally, as compelling evidence of the technological potential of the silicene membranes, it is demonstrated that they can be readily introduced into a lithographic process flow resulting in the definition of flexible device‐ready architectures, a piezoresistor, and thus paving the way to a viable advance in a fully silicon‐compatible technology framework.

Silicene or two-dimensional (2D) graphene-like silicon allotrope has recently emerged as a promising candidate for various applications in nanotechnology. However, few concerns involving its stability persist to date and need...