The catalytic activity of the perovskite-like layered oxides NaNdTiO 4 , LiNdTiO 4 , and НNdTiO 4 in the reaction of the methyl orange dye decomposition under the action of UV irradiation was studied. Rate constants of the pseudo-first order were determined. It was found that in the series NaNdTiO 4 , НNdTiO 4 , and LiNdTiO 4 the photocatalytic activity of the layered oxides increases.Recently the possibility of using complex layered oxides (titanates, tantalates, and niobates) as catalysts of photoinduced processes is actively studied [1,2]. Complex oxides of rare-earth and alkaline elements are considered as an alternative to binary oxides, in particular, to widely known and effective photocatalyst, titanium dioxide. The attractiveness of the complex oxides consists in a possibility of varying cationic composition, thus influencing their catalytic activity. Moreover, in complex oxides with a layered structure the intercalation of water molecules in the interplanar space [3, 4] is possible, which can be considered as an increase in the effective specific surface area of a photocatalyst. At present the effect of the nature of the interlayer space on the photocatalytic activity is insufficiently studied. Also experimental data are deficient on the photocatalytic activity of isostructural layered oxides in decomposition reactions of organic substances under identical conditions.In this work we present the results of the study of photocatalytic activity of layered perovskite-like oxides with a similar structure, but different cationic composition. The comparative analysis of the photocatalytic activity of oxides has been fulfilled using the reaction of photoinduced decomposition of the methyl orange dye under UV irradiation.The layered complex oxides NaNdTiO 4 , HNdTiO 4 , and LiNdTiP 4 belong to cation-ordered RuddlesdenPopper phases and are built according to a block principle by jointing layers with the perovskite structure and fragments with the NaCl structure. In the structure of the oxides under consideration variously charged cations are completely ordered in different layers of the layered structure because of essential differences in sizes and charges of Nd +3 cations and cations of alkali metals (Na +1 , Li +1 ) or a proton. It is the reason which is responsible for the possibility of the synthesis of НNdTiO 4 and LiNdTiO 4 by ionexchange reactions from NaNdTiO 4 , which can be obtained by a high-temperature solid-phase synthesis.According to the X-ray analysis, samples of NaNdTiO 4 , HNdTiO 4 , and LiNdTiO 4 oxides, which were used for the study of catalytic activity, were monophase. According to the electron microscopy data, the particle size of layered titanates essentially exceeds that of titanium dioxide (50 nm) used for their synthesis. It is connected with the fact that NaNdTiO 4 was obtained by a ceramic method, which is characterized by the enlargement of particle sizes of synthesis products, as compared with reagents, due to caking at a high temperature. Particles of the complex oxides NaNdTiO 4 ...