Coupling membrane filtration with photocatalysis provides multifunction involving filtration and photocatalytic degradation for removing pollutants from water, but the performance of photocatalytic membrane is limited due to the quick recombination of photogenerated electron-holes in photocatalytic layer. Herein, a TiO2/carbon/Al2O3 membrane was designed and constructed through sequentially depositing graphitic carbon layer with good electro-conductivity and TiO2 nanoparticles layer with photocatalytic activity on Al2O3 membrane support. When light irradiated on the membrane with a voltage supply, the photogenerated electrons could be drained from photocatalytic layer and separated with holes efficiently, thus endowing the membrane with photoelectrocatalytic function. Membrane performance tests indicated that the photoelectrocatalytic membrane filtration (PECM) showed improved removal of natural organic matters (NOMs) and permeate flux with increasing voltage supply. For PECM process at 1.0 V, its NOMs removal was 1.2 or 1.7 times higher than that of filtration with UV irradiation or filtration alone, and its stable permeate flux was 1.3 or 3 times higher than that of filtration with UV irradiation or filtration alone. Moreover, the PECM process exhibited special advantage in removing organic chemicals (e.g., Rhodamine B), which displayed 1.3 or 3 times higher removal than that of filtration with UV irradiation or filtration alone.