Groundwater is being depleted globally at an average rate of more than one meter per year, during a period when more than a quarter of the human population has no access to potable water. Aside from overexploitation, freshwater security is also threatened by climate change and chemical pollution. The contamination of surface and groundwater by industrial substances is also undermining the vitality of ecosystems. It was previously shown that {100}-faceted Bi2MoO6-Laponite hybrids effectively bind and photodegrade molecular species, aiding in the decontamination of water. In this study, the encapsulation of Bi2MoO6-Laponite particles with the polymers butyl acrylate and styrene further enhanced adsorption of methylene blue by 31.4%, with a specific adsorption capacity of 192 μmol/g. The polymer-particle composites were deposited to form membranes and their efficacies in water filtration and photodegradation were examined. Among the different surface modifications examined, the highest dye sorption was obtained by butyl acrylate and styrene (3:2) with a 5 mol % cross-linker. This study provides a method for enhancing the molecular adsorption of composite particles used in membranes capable of multiple cycles of adsorption and photodegradation, advancing the application of such systems to water filtration.