Nanosized titanium dioxide (TiO2)-based materials are regarded as an effective approach for disposing organic pollutants. However, their wide bandgap, rapid electron/hole recombination, poor chemisorption, and aggregation limit their photoactivity and photocatalytic efficiency. In this study, the coupling of TiO2 and a conjugated polymer membrane is created to improve the photoactivity and photocatalytic efficiency of TiO2. Nanosized TiO2 with high crystallinity is synthesized on the surface of the pretreated poly(phenylene sulfide) (PPS) porous membrane through the in situ hydrothermal process. Strong interaction forms between the prepared TiO2 and the membrane matrix, which leads to the efficient migration and transfer of electron-hole pairs. As a result, the band gap and the electron/hole recombination rate of TiO2 significantly decrease. The TiO2@PPS membrane possesses better adsorption capacity compared with the photocatalyst consisting of individual TiO2, which will greatly increase the photocatalytic efficiency. Various dyes can be degraded almost completely after being irradiated for 90 min under visible light. In a word, it may provide a facile approach for preparing a photocatalytic membrane with a high catalyst loading amount, a large chemisorption capacity, and high visible-light photoactivity.