A 10 L membrane bioreactor (MBR) was constructed with novel iron-tannin-framework ultrafiltration membrane (ITUM) for membrane fouling mitigation and effluent quality improvement. Compared to commercial ultrafiltration membrane (CUM) in the same MBR, ITUM exhibited hydrophilicity with a contact angle of 64.18° (71.36° for CUM), resulting the permeance of ITUM (50.2 L m-2h−2 bar−1) 1.8 times higher than CUM. During 70-day operation, ITUM was consistently run at lower transmembrane pressure. After operation, the polyethersulfone (PES) peak intensity of ITUM reduced less than 1 % (85 % for CUM), which indicated a thinner sludge layer on ITUM. Meanwhile, the average effluent chemical oxygen demand concentration for ITUM and CUM achieved 16.69 and 17.60 mg L-1 in stable phase, respectively. For NH4+-N, it could reach 0 and 0.04 mg L-1. 16 s RNA results showed that Saccharibacteria accounted for 1.48 % and 1.20 % on ITUM and CUM, respectively. According to first-principles density functional theory simulations, simulated adsorption energies was −1.330 eV for gram-positive bacteria (such as Saccharibacteria). It was −0.867 eV for Fe(Ⅲ) to gram-negative bacteria. It suggests that ITUM could easily attract microorganisms with the ability of polysaccharide degradation, while reducing this type of pollutants deposition on membrane. Therefore, the ITUM received a more superior effluent quality and membrane fouling resistance.