To address the increasing interest in environmental issues, green and sustainable material-based membranes have attracted significant research interest with the promise to replace fossil-based membranes and to reduce waste generation. In this work, more sustainable thin-film composite (TFC) membranes are designed and fabricated via interfacial polymerization of green building blocks, namely, shrimp farming waste chitosan in the aqueous phase and plant-based 2,5-furandicarboxaldehyde in the organic phase, on an upcycled polyethylene terephthalate porous support. The TFC membranes showed excellent acetone permeance up to 12 L m–2 h–1 bar–1 with a molecular weight cutoff value of approximately 317 g mol–1. The membrane separation performance was optimized by fine-tuning the building block concentrations, which provided a new upper-bound in the plot of acetone permeance versus styrene dimer rejection. In addition, for the first time, TamiSolve was employed as a green solvent to activate the selective layer of the chitosan-based TFC membrane, resulting in a significant enhancement in the permeance of diverse pure solvents including ethanol, methyl ethyl ketone, acetone, and acetonitrile with no remarkable defects and high solute rejections. Our proposed green TFC fabrication platform enables the replacement of toxic and fossil-based solvents and reagents in developing high-performance and solvent-resistant nanofiltration membranes.