In order to utilize sustainable solar energy, cyclic operations of syngas production by methane reforming (reduction) and subsequent hydrogen production by water splitting (oxidation) were performed by using simulated solar-light irradiation to ZrO2-supported CeO2 particles which were coated on a SiC ceramic foam disk. This redox process is a promising chemical pathway for storage and transportation of solar heat by converting solar energy to chemical energy. By properly adjusting the methane reforming time, carbon deposition due to the undesirable methane decomposition could be avoided. The produced syngas had the H2/CO ratio of 2.0, which is suitable for the Fischer–Tropsch synthesis or methanol synthesis, and the produced pure hydrogen can be used for fuel cells. When the cyclic reactions were repeated several times at two temperatures (800 °C, 900 °C), the conversion of CeO2 and the H2 yield were reasonable and were maintained nearly constant from the second cycle, exhibiting good stability of the redox process.