In the present study we report on the activity, selectivity and stability of the bimodal mesoporous NiO/CeO2-delta-YSZ anodes for IT-SOFCs applications. These materials present high concentration of C3+ ions stably retained in the lattice, which proved to be efficient for the catalytic partial oxidation of CH4 to syngas in the temperature range 600-800 degrees C. The excellent carbon tolerance was proved by a comprehensive XPS analysis, which monitored the amount of carbon before and after catalytic partial oxidation of methane (CPOM) tests. The mesoporous anodes templated by hexadecyltrimethylammonium bromide (CTAB) and tripropylamine (TPA) were obtained using a hydrothermal synthesis route. The effect of Ni and Ce incorporation on the yttria stabilized zirconia (YSZ) structure, texture, morphology and surface chemistry was discussed and correlated with catalytic and electrochemical behavior. The exhaustive characterization of the bulk and surface properties of the catalysts have been accomplished by means of complementary methods: XRD, SEM / EDX / HR TEM, TGA / TPR, XPS. The electrochemical and catalytic performance were improved when the surface contains more reduced ceria and NiO was formed as secondary phase. These features lead to a large number of vacancies and consequently a better oxygen migration, which facilitate the carbon removal.