H2NiTi4O10/TiO2 intercalated compound was fabricated by successive intercalation reactions of H2NiTi4O10 with n-C6H13NH2/C2H5OH mixed solution and acid TiO2 sol, followed by irradiating with a high-pressure mercury lamp. H2NiTi4O10, a layered perovskite type compound with TiO2-loading, exhibited a high activity for decomposition of methyl orange under UV and visible light irradiation. The experimental results showed that methyl orange was degraded with the decomposition ratio of 59.0 % by using H2NiTi4O10/TiO2 as photocatalyst under visible light ( > 420 nm) irradiation for 24 h. The H2NiTi4O10/TiO2 possessed higher photocatalytic activity than those commercial titania powder (Degussa P-25) which showed the decomposition ratio just only 24% under same condition.