A new ex-TTF-based organogelator with l-glutamide-derived lipid unit (compound 1) was synthesized and characterized. The resulting transparent organogels can be obtained with several organic solvents such as toluene, DMSO, and ethanol. It is interesting that its gelation ability can be further enhanced by addition of C-60. The H-1 NMR and absorption spectral studies indicate that the intermolecular interaction between the ex-TTF unit in 1 and C-60 may be responsible for this phenomenon. Further studies imply that the assembly structures in the gel phases in the absence and presence of C-60 may be different. Additionally, organogels can also be prepared with compound 1 and PCBM, and the corresponding xerogel was used to modify ITO electrode. A stable and rapid photocurrent was generated after exposure of the modified ITO electrode to light. This may provide an alternative way for photocurrent generation with high energy conversion efficiency.