Polysulfone (PSf) composite ultrafiltration membranes were subjected to Ar/O₂ plasma assisted oxygen activation and then coated with various forms of metallic glass (W₅₀Ni₂₅B₂₅, Zr₆₀Cu₂₅Al₁₀Ni₅, and Pd₇₄Si₁₄Cu₁₂). The activated oxygen treated PSf ultrafiltration membrane was strongly hydrophilic, with pure water flux (PWF) of 350.7 L m⁻² h⁻¹ and bovine serum albumin (BSA) rejection of 83%. The application of metallic glass (MG) to the surface of the polysulfone composite membrane using low-power radio-frequency magnetron sputtering improved the BSA rejection rate (ranging from 98.6 to 99.9%) with only a slight reduction in PWF: tungsten-based MG (321.5 L m⁻² h⁻¹), zirconium-based MG (215.6 L m⁻² h⁻¹), and palladium-based MG (181.3 L m⁻² h⁻¹). The membrane with the tungsten-based coating achieved remarkable PWF, BSA rejection, and antifouling performance, due primarily to high surface hydrophilicity (water contact angle of 24.2°) and a strongly negative surface charge. Overall, the proposed metallic glass/polysulfone composite membranes achieved moderately high PWF and protein rejection with incredible antifouling competence, even under extended (multi-cycle) fouling conditions.