On the basis of combinatorial methodology and the idea of an equilateral ingredient triangle, the TiO(2)/ZnO/Fe(2)O(3) composite system including 66 ingredient points was designed. The photocurrents under different light sources and bias voltages were measured, and the photocurrent amplitude at 300 s was chosen as a parameter to evaluate the photoelectric response of the composite. To appraise the composition effect of the composite compared with pure materials, the quantitative formula of the composition effect has been provided for the first time in this paper. We found that not all the ingredient points demonstrated the enhanced composition effect in the as-designed ingredient triangle material library. The reasons of different composition effect for different ingredient points have been discussed in detail. X-ray diffraction (XRD) and field emission scanning electron microscopy (FE-SEM) were used to investigate the phase structure and the grain morphology of the composite.