The pi-pi stacking of self-assembled PTCDI and pi-pi interactions between self-assembled PTCDI and C-60 result in fast transfer of the photogenerated carriers and reduced carrier recombination. The pi-pi interaction lowers the position of valence band and narrows the band gap, thus leading to a stronger redox ability and a broad spectral response. The organic photocatalyst PTCDI-C-60 can not only degrading phenol at a rate of 0.216 h(-1), which is 8.24 times higher than that of pure PTCDI, but also producing oxygen at a rate of 22.5 mu mol g(-1) h(-1). Moreover, the presence of C-60 stabilizes the composite to decrease the accumulation of negative charge. The high catalytic activity can potentially be utilized in the fields of environmental and energy applications.