Humanity has an urgent need to develop more degradable materials for solving environmental pollution. In this study, through host–guest interactions between fatty acids-modified β-cyclodextrin (Em-βCD) and polyethylenimine (PEI) oligomer-grafted ferrocene (PEI-Fc), we designed and prepared a supramolecular polymer (PEI-Fc/Em-βCD complex), which showed polymeric properties and was able to be used as a cushioning material due to its good compressibility. Compared with conventional polymers, a remarkable advantage of the PEI-Fc/Em-βCD complex is that it can be dismantled into small molecules and rebuilt easily by controlling the dissociation or reformation of βCD-Fc inclusion complexes. Furthermore, the material also exhibited good self-healing properties.