In this study, a novel membrane bioreactor (MBR) inoculated with algal-bacterial granular sludge (ABGMBR) was established to improve pollutant removal and alleviate membrane fouling. The ABGMBR system showed higher pollutant removal rate and longer operation time (152 day) compared to the control MBR (AGMBR). Moreover, the contents of the pollutants such as granular sludges, extracellular polymeric substances (EPS), and soluble microbial products on the membrane were remarkably reduced, leading to the formation of a porous and loose cake layer on the membrane and a slow increase in transmembrane pressure. Standard blocking was the main mechanism of membrane fouling; however, the membrane pore blockage was significantly reduced in ABGMBR. The extended Derjaguin-Landau-Verwey-Overbeek (XDLVO) theory suggested that the aggregation and adhesion of foulants on the membrane were greatly inhibited in ABGMBR. Furthermore, correlation analysis showed significant differences in membrane fouling characteristics between AGMBR and ABGMBR. The ABGMBR system effectively retarded sludge disintegration and increased the repulsion between the sludge and membrane owing to the favorable mixed liquor characteristics. This study showcases the superior operational efficiency and anti-fouling performance of ABGMBR, offering a novel perspective on sewage reuse and membrane fouling mitigation.