The application of electrochemistry or photochemistry to modulate supramolecular interactions between host–guest systems in solution is a burgeoning field. In particular, the speed and reversibility associated with electrochemically or photochemically actuated supramolecular interactions has allowed the creation and modulation of novel solution‐based devices. In recent years, great advances have been made in transferring these systems from the solution to the solid state, to facilitate the development of molecular‐electronics components that can operate in unison under the influence of an externally applied stimulus. These studies pave the way for the creation of responsive surfaces with advanced materials and nanotechnology applications. Solid progress: The transfer of responsive supramolecular systems from the solution to the solid state by immobilizing their components onto surfaces is an attractive method for developing systems with molecular electronics and device applications (see scheme). The ability to coherently interface these systems with the outside world may pave the way for their implementation as novel components within the emerging advanced materials and nanotechnology industries.