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In present study,a simultaneous electrospinning and electrospraying (SEE) process was employed to produce microclusters of TiO2 nanoparticles and interlock them in nanofibrous network.The photocatalytic composite membranes (PCMs) were fabricated by electrospraying TiO2 nanoparticcle suspension into microususter form that dispersed and entrapped within nylon-6 electrospun fiber membrane.Three PCMs membrane with TiO2 content of 52.0,83.6,and 91.7 wt.％ were successfully fabricated.The membrane consisted of TiO2 microclusters,ranging in sizes from around 0.3 to 10 μm,distributed uniformly within the nylon-6 nanofibrous network.PCMs photocatalytic activity against Methylene Blue (MB) in aqueous solution showed more than 98％ MB removal efficiency after 120 min of photocatalytic oxidation (PCO) for all PCMs.For PCM with the highest TiO2 content tested for 5 PCO cycles,it was found that most of their TiO2 content remained incorporated Within the nanofibrous structure.The concept of nanoparticles clusters entrapment with SEE fabrication employed here provide a simple and effective method for reducing detachment of nanostructure phase from nanocomposite membrane.