Rotaxane-based molecules have been intensively studied for use as functional molecular electronic devices and as a medium for nanorecording. By means of both I-V, Raman and conductive contact atomic force microscopic measurements of rotaxane H1 and H2 molecular thin films and scanning tunneling microscopy studies of individual H2 molecules, we demonstrate conclusively that the conductance transition originates from single molecules and correlates with changes in molecular conformation. This provides the best evidence to date that the conductance transition arises from motion of the cyclobis(paraquat-p-phenylene) ring along the molecular backbone. Taking advantage of the switching property, we have achieved reproducible nanometer-scale recording (dots) on rotaxane Langmuir-Blodgett (LB) films via voltage application using a scanning tunneling microscope (STM) probe. Stable, reversible conductance transitions and memory effects were observed in solid state rotaxane-based H1 LB thin films; while the thin films of rotaxane H2 molecule can be successfully written, erased, re-written, and re-erased. The stable and controllable conductance switching makes the rotaxane an attractive candidate for nanorecording. Furthermore, these results suggest that controlling the rotaxane conformation, its electronic structure, and decoration of the molecule, are strongly needed to strive the practical applications to the molecular electronic devices.