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To meet the urgent need of society for advanced photocatalytic materials, novel visible light driven heterostructured composite was constructed based on graphitic carbon nitride (g-C3N4) and fibrous TiO2. The g-C3N4/TiO2 (CNT) composite was prepared through electrospinning technology and followed calcination process. The state of the g-C3N4 and fibrous TiO2 was tightly coupled. The photocatalytic performance was measured by degrading the Rhodamine B. Compared to commercial TiO2 (P25®) and electrospun TiO2 nanofibers, the photocatalytic performance of CNT composite was higher than them. The formation of CNT heterostructures and the enlarged specific surface area enhanced the photocatalytic performance, suppressing the recombination rate of photogenerated carriers while broadening the absorption range of light spectrum. Our studies have demonstrated that heterostructured CNT composite with an appropriate proportion can rational use of visible light and can significantly promote the photogenerated charges transferred at the contact interface between g-C3N4 and TiO2.