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Strain-driven micro- and nanorolls fabrication is generally restricted to multilayer and multiprocessing systems, which limit the possibility of exploiting the self-organization at different length scales. We have designed a hybrid organic–inorganic film whose surface shows a selective response to external stimuli, which induces mechanical strain and self-rolling in one-step–one-layer fabrication. The scrolling is initiated by water and any aqueous solution that also contains molecules or colloidal particles. During scrolling, the different species in solution remain entrapped in the rolls, giving rise to functional microrolls.
