Induced surface reconstruction of silicone rubber by blending polydimethylsiloxane (PDMS) reactants with bifunctional PDMS-hydroxyl terminated polybutadiene (PDMS-b-HTPB) copolymers and curing with appropriate mold material was attempted to improve the adhesion of chemically inert silicone rubber to polyurethane (PU). Surface characterization using Fourier transform infrared-attenuated total reflectance indicated that the surface of the silicone rubber possessed a controlled amount of HTPB. The surface was enriched with HTPB by using mold materials having high critical surface tension, such as aluminum. A dynamic surface rearrangement occurred during a l-h heating cycle at 70 degrees C, changing from an HTPB-enriched surface to a PDMS-enriched surface. The peel strength between the silicons rubber and PU was found to increase with decreased propanol residue and with an increase in critical surface tension of the molding materials. The increased content of surface HTPB was suggested to account for the improved adhesion of silicone rubber to PU.