The structure and mechanical properties of polybutadiene (PB) films on bare and surface-modified carbon films were examined. There was an interfacial layer of PB near the carbon layer whose density was higher (lower) than that of the bulk material on the hydrophobic (hydrophilic) carbon surface. To glean information about the structure and mechanical properties of PB at the carbon interface, a residual layer (RL) adhering to the carbon surface, which was considered to be a model of "bound rubber layer", was obtained by rinsing the PB film with toluene. The density and thickness of the RLs were identical to those of the interfacial layer of the PB film. In accordance with the change in the density, normal stress of the RLs evaluated by atomic force microscopy was also dependent on the surface free energy: the RLs on the hydrophobic carbon were hard like glass, whereas those on the hydrophilic carbon were soft like rubber. Similarly, the wear test revealed that the RLs on the hydrophilic carbon could be peeled off by scratching under a certain stress, whereas the RLs on the hydrophobic carbons were resistant to scratching.