Vertically-aligned, self-assembled carbon-Fe:TiO2 hybrid nanobelts were synthesized using a simple and low-cost metalorganic chemical vapor deposition (MOCVD). Residual C, a by-product of MOCVD reaction, was utilized to form a nanographitic layer at the tip of the nanobelts, by which the Fe:TiO2 nanobelt growth was mediated as the growth temperature was determined judiciously at 510 degrees C. The Fe:TiO2 coating on the nanographitic layer is governed by Volmer-Weber and step-flow growth modes. The resultant vertically-aligned C-Fe:TiO2 hybrid nanobelts have significant potential for various photocatalysis, solar cell, and Li-ion battery applications.