This work has been focused on the one-step fabrication by electrospinning of polyamide 6 (PA6) nanofibre membranes modified with titanium dioxide nanoparticles (TiO2), where these TiO2 nanoparticles aggregates could induce a photocatalytic activity. The main potential application of these membranes could be the purification of contaminated water. Thus, it is important to analyse the contaminant degradation capability since in these membranes this is based on their photocatalytic activity. In this work, the effect of the photocatalysis has been studied both on the degradation of an organic model contaminant and on the removal of Escherichia coli and other coliform bacteria. As a result, it was observed that these membranes present excellent photocatalytic activity when they are irradiated under UV light, allowing a 70% reduction of an organic model pollutant after 240 min. In addition, these membranes successfully removed Escherichia coli and other coliform bacteria in artificially inoculated water after 24 h of contact with them. Moreover, the stand-alone structure of the membranes allowed for the reusing of the immobilized catalyst. The experimental evidence indicated that developed nanofibre membranes are a fast and efficient solution for polluted water decontamination based on photocatalysis. Their use could contribute to guarantee a fresh water level and quality, mitigating the water scarcity problem worldwide.