We studied enhanced interfacial adhesion between an amorphous polymer (polystyrene, PS) and a semicrystalline polymer (a polyamide, Ny6). The fracture mechanism for this system was investigated to elicit a universal description on the fracture mechanism. The surface modification of PS to provide functional groups that can react with the functional groups of Ny6 was carried out with ion-beam and/or plasma treatment. These surface modifications were found to alter the interfacial adhesion strength between PS and Ny6. A remarkable enhancement was found with the surface functionalization of PS. Though the fracture toughness was varied depending on the process, its overall behavior was quite similar to that of others; the fracture toughness increased with increasing bonding temperature and bonding time, passed through a peak, and then decreased with a further increase of the bonding time or temperature. The variation of the fracture toughness with the bonding time and temperature can be plausibly explained in terms of two different failure mechanisms of adhesive failure and cohesive failure. This change appears more evidently for the interface between an amorphous polymer and a semicrystalline polymer than the interface between semicrystalline polymer pairs. Surface functionalization could exclude the effect of diffusion, thus clarifying the failure mechanisms occurring at the interface.