An organic-inorganic layered hybrid was prepared by intercalation of Fe(bPY)(3)(2+) into laponite clay. UV-vis diffuse reflectance, X-Ray diffraction, and SEM confirmed the intercalation and the strong host-guest interaction of Fe(bpY)(3)(2+) molecules with the clay matrix. Compared with laponite, the hybrid formed a solid layered structure due to the linking of laponite platelets by Fe(bpy)(3)(2+) molecules. Upon visible light irradiation (gimel > 420 nm), the hybrid was found to be highly effective for the degradation of nonbiodegradable cationic organic pollutants such as Rhodamine B (RhB) and N,N-dimethylaniline by activating H2O2 at neutral pH values, but inactive toward anionic organic compounds such as Orange II and Sufforhodamine-B. The adsorption and degradation of organics on the hybrid could be controlled by changing the pH value of the suspension. The total organic carbon (TOC) removal yield of RhB was 41%. pH effect trials and the final degraded products further indicate that unless the target is adsorbed onto the clay layers the reaction could not occur. Neither (OH)-O-center dot nor (OOH)-O-center dot/O-2(center dot-) EPR signals were detected during the reaction. The solid support of laponite not only alters the photochemical properties of Fe(bpY)(3)(2+) but also provides a rigid microenvironment for the enrichment of local substrate molecules and thus enhances the interaction of the active center with the substrate. (c) 2006 Elsevier B.V. All rights reserved.