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From analyses of pressure−area isotherms and X-ray photoelectron spectra, we have demonstrated that redox-controllable molecular shuttles, in the shape of amphiphilic, bistable rotaxanes, are mechanically switchable in closely packed Langmuir films with chemical reagents. Additionally, mechanical switching has been proven to occur in closely packed Langmuir−Blodgett bilayers while mounted on solid substrates. The results not only constitute a proof of principle but they also provide the impetus to develop solid-state nanoelectromechanical systems that have the potential to reach up to the mesoscale.