Composite films of different molecular weight poly(phenylene sulfide) (PPS) and three types of carbon fibers (Pitch, PAN, and Rayon-based fibers) have been studied by optical microscopy and wide-angle X-ray diffraction. Transcrystallization of growing spherulites on carbon fibers is found under all thermal conditions of growth on Rayon and Pitch-based carbon fibers for all types of matrices. For composite films with PAN carbon fibers transcrystallization of growing spherulites is not uniform and sometimes is not found at all. Existence of b axial orientation of twisted lamellae for transcrystalline zone of PPS is demonstrated by X-ray diffraction technique and compared with orientation of the stretched sample. The new induction time quantitative approach is applied to the transcrystalline growth of PPS spherulites on the surface of carbon fibers. The interfacial free energy difference for fiber/crystallite and heterogeneities/ crystallite systems in the melt that is defined from growth and nucleation studies are calculated and compared. The relative tendency for a polymer to crystallize at the fiber surface rather than in the bulk is demonstrated.