The effective separation of dyes and inorganic salts is highly desirable for recycling inorganic salts and water resource in printing and dyeing wastewater treatment. In this work, tannic acid (TA) and polyethyleneimine (PEI) were grafted on the PES/Fe ultrafiltration membrane via the coordination assembly and Michael addition strategy to fabricated a loose nanofiltration membrane (LNM). The effect of PEI concentration on membrane morphologies and properties was systematically investigated. The membrane surface becomes more hydrophilic and transforms into positive charge after the PEI grafting. The optimized PES/Fe-TA-PEI membrane possesses high pure water flux (124.6 L·m−2·h−1) and excellent dye rejections (98.5%, 99.8%, 98.4%, and 86.4% for Congo red, Eriochrome black T, Alcian blue 8GX, and Bromophenol blue, respectively) under 2 bar operation pressure. Meanwhile, the LNM showed a high Alcian blue 8GX rejection (>98.4%) and low NaCl rejection (<5.3%) for the dye/salt mixed solutions separation. Moreover, the PES/Fe-TA-PEI LNM exhibited good antifouling performance and long-term performance stability. These results reveal that such LNM shows great potential for effective fractionation of dyes and salts and recycling of textile wastewater.