In response to the above research needs, we propose a facile LbL approach to deposit TiO2 and GO on a polysulfone (PSf) base membrane to enable photoactivity under both UV and sunlight. After the deposition phase, stable bonding between GO and TiO2 layers was created by post-treating the membrane with ethanol and UV. We verified the effectiveness of the LbL procedure by quartz crystal microbalance with dissipation (QCM-D) and char- acterized the properties of the TiO2–GO membrane by various techniques. Finally we tested the performance (i.e., water flux, photodegradation of organic dyes) of the TiO2–GO membrane under different light sources.