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Abstract In this study, loose nanofiltration membranes made of polysulfone dissolved in co-solvents PolarClean and gamma-Valerolactone were prepared via slot die coating (SDC) on a roll-to-roll (R2R) system by directly coating them onto a support layer or free standing. A solution flow rate of 20 mL/min, substrate speed of 17.1 mm/s, and coating gap of 0.1 mm resulted in the formation of membranes without structural defects. Pre-wetting the support layer with dope solution minimized shrinkage of membrane layer thickness and improved interfacial adhesion. Membrane samples produced using SDC exhibited properties and performance consistent with bench-scale doctor blade extruded samples; pre-wetted and uncompressed samples (SDC-3) exhibited the highest rejection of bovine serum albumin (99.20% ± 1.31%) and along with adequate mean permeability during filtration (70.5 ± 8.33 LMH/bar). This study shows that combining sustainable materials development with SDC provides a holistic approach to membrane separations to bridge materials discovery and membrane formation.