The　key　to　achieve　sustainable　treatment　of　high-salinity　dye-containing　wastewater　is　effective　fractionation　of　dyes　and　salts.　In　this　study,　a　thin-film　composite　electro-nanofiltration　membrane　was　successfully　fabricated　by　co-deposition　of　levodopa　and　ε-polylysine　onto　a　porous　ultrafiltration　membrane　substrate.　With　the　co-deposition　of　the　polylevodopa/ε-polylysine　composite　coating　on　the　substrate　membrane,　the　surface　properties　were　significantly　regulated,　resulting　in　decreased　pore　size,　reduced　surface　negative　charge　density　and　lower　specific　electric　resistance,　thus　enhancing　their　ion　transfer　and　dye/salt　fractionation　efficacy.　Specifically,　the　fabricated　LDP-4　membrane　(molecular　weight　cut-off　of　408　Da)　with　a　4-h　co-deposition　experienced　a　99.12　%　reactive　orange　16　dye　rejection　and　10.15　%　NaCl　rejection,　indicating　an　impressive　selectivity　between　dyes　and　salts.　Additionally,　the　LDP-4　electro-nanofiltration　membrane　as　anion　conducting　membrane　exhibited　a　fast　and　efficient　electro-driven　transfer　of　Cl−　ions.　Notably,　under　an　electric　field,　the　fabricated　LDP-4　electro-nanofiltration　membrane　can　efficiently　fractionate　NaCl　from　the　reactive　orange　16/NaCl　mixed　solution,　achieving　a　98.89　%　desalination　efficiency　and　99.79　%　dye　recovery.　Furthermore,　the　LDP-4　membrane　demonstrated　remarkable　anti-fouling　property　and　long-term　stability　over　an　8-cycle　electro-nanofiltration　operation.　Therefore,　the　electro-nanofiltration　membranes　fabricated　by　co-deposition　of　levodopa　and　ε-polylysine　show　a　promising　potential　in　sustainable　resource　recovery　from　high-salinity　dye-containing　wastewater.　©　2024　Elsevier　B.V.