For polymer composites, interfacial crystalline structures retain an important role in the macroscopic properties and are significantly affected by the processing conditions, such as the temperature, time, and external field. In this study, the transcrystallization behavior of the carbon nanotube fiber and isotactic polypropylene composite was investigated by polarizing light microscopy. The influence of the formation of the transcrystalline layer on the interfacial adhesion was evaluated by a single-fiber fragmentation test. The results show that the growth rate of the transcrystalline layer was strongly influenced by the isothermal crystallization temperature, and the interfacial shear strength was markedly enhanced by the formation of the layer. The interfacial adhesion was further increased with the gradual perfection and growth of transcrystallinity.