Centrifugal slurry-pouring method has been proposed to fabricate the functionally graded materials (FGMs) with large compositional gradient. This processing method uses the two types of slurries (slurry 1 and slurry 2). The prepared slurry 1 containing one component, particle A, is firstly poured into the mold under the centrifugal force and then the slurry 2 containing two components, particle A and particle B, is poured into the mold. By this process, green body with gradient composition can be obtained and then green body will be sintered by Spark Plasma Sintering method. Finally, it is expected that FGM with gradient from 100% component A at one surface to 100% B at other surface can be fabricated. In this study, the graded distributions of the particle A and particle B within the slurry 2 under the centrifugal force were simulated analyzing the movement of particles in liquid. Moreover, Ti-SiO2 FGMs were experimentally fabricated. The Ti-SiO2 FGM has large compositional gradient on one side of FGM. However, when the size of solid-particle is small, it is difficult to form large compositional gradient in the FGM. This phenomenon obtained by experiment is in agreement with the calculated results. From this result, it is found that the centrifugal slurry-pouring method using different slurries is effective fabrication method for FGMs with large compositional gradient.