Photodegradation of an organic dye was studied experimentally using novel polymer-titania microcomposites. These microcomposites were prepared from titanium dioxide (TiO2) nanoparticles embedded within cross-linked, thermally-responsive microgels of poly(N-isopropylacrylamide) and contained interpenetrating linear chains of poly(acrylic acid) that functionalize the nanoparticles of TiO2. Because these microcomposites settle more than a hundred times faster than freely suspended TiO2 nanoparticles, they are extremely useful for simple gravity separation of the photocatalyst in applications that employ titania nanoparticles. Methyl orange (MO) was used as a model contaminant to investigate the degradation kinetics using the microcomposites in aqueous suspensions. Kinetics of the photodegradation were evaluated by monitoring the changes in methyl orange concentration using UV-Vis spectroscopy. The photocatalytic behavior of functional microcomposites containing 65 wt% titania was studied and the influence of the solution pH as well as the total titania concentration in solution was explored. The results indicated that pH of the solution changes the surface interactions between the poly(acrylic acid), titania, and methyl orange and this interplay determined the overall degradation kinetics of the chemical contaminants. Nearly identical reaction rate constants were observed in acidic solutions for the microcomposites when compared to freely suspended titania. The latter showed higher rate constants than the microcomposites at a neutral pH. Release of the titania from the microcomposites was observed under basic conditions. Complete degradation of the microcomposites was observed after prolonged (713 h) UV irradiation. However, the microcomposites were easily regenerated by addition of microgels and no loss of photocatalytic activity was observed. (C) 2009 Elsevier Inc. All rights reserved.