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New polyoxometalate (POM)/polymer hybrid composites were prepared by photopolymerization under mild conditions for suitable photocatalytic processes. Polyoxometalates were incorporated in special photosensitive resins, which were photopolymerized under visible light to obtain new materials with photocatalytic activity for dye removal. The synthesized composites were characterized by real‐time FT‐IR, and the photocatalytic ability was investigated on Eosin‐Y removal using photolysis under near UV irradiation. Interestingly, the polyoxometalates keep their photocatalytic properties, while incorporated into the polymeric matrix since very high conversion rates of Eosin‐Y were achieved. Indeed, degradation efficiencies of about 98% and 93% were registered when using H3PMo12O40/polymer and 94% for SiMo12O40(IPh2)4/polymer composites, respectively. These first results reported in this article show that the new synthesized POM/polymer composites could be considered as promising materials for green and more suitable organic dye removal from aqueous solutions. © 2019 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2019, 57, 1538–1549 [ABSTRACT FROM AUTHOR]