A novel "sliding graft copolymer" (SGC), in which many linear poly-ε-caprolactone (PCL) side chains are bound to cyclodextrin rings of a polyrotaxane, was prepared by ring-opening polymerization of ε-caprolactone initiated by hydroxyl groups of the polyrotaxane. An amorphous, flexible, and sufficiently tough elastomer film was prepared by crosslinking the obtained SGC-a supramolecule possessing a number of mobile side chains-with hexamethylene diisocyanate (HMDI).