Wrinkled structures can provide enlarged surface areas for some living organisms to ingest nutrients. Imitating biological wrinkle structures offers an efficient way to enhance the adsorption surface for removing hazardous pollutants in wastewater. In this work, poly-(ethylene glycol) double acrylate (PEGDA)/TiO2 composite film with tunable surface wrinkles was synthesized. TiO2 nanoparticles were evenly immobilized in the PEGDA hydrogel simply by a facile photopolymerization method within 700 ms. Various wrinkle morphologies were obtained by precisely controlling UV exposure time. The composite film was characterized by X-ray diffraction, scanning electron microscopy, diffuse reflection spectroscopy, etc. Congo red was chosen as a model pollutant to demonstrate the adsorption and degradation capacity of the composite film. The experimental results showed that the introduction of wrinkled polymer improved the dispersibility of TiO2 nanoparticles. The removal efficiency reached 100% after 180-min adsorption in the darkness and 180-min UV irradiation. The composite film exhibited a much higher enrichment and photocatalysis capacity than the pure TiO2 powder, and could be developed as a reusable film for the removal of the organic pollutants in wastewater. (C) 2018 Elsevier B.V. All rights reserved.