The high-salinity wastewater from the textile industry faces a significant challenge in effectively separating dyes and salts. In this study, a CeZnFe-layered double hydroxide (LDH)-incorporated nanofiltration (LNF) membrane was fabricated using the conventional interfacial polymerization (IP) technique to fractionate dyes and salts within the wastewater. The impact of CeZnFe LDH on various aspects of membrane performance was examined, including water flux, dye removal efficiency, dye/salt separation capability, self-cleaning ability, and membrane integrity. The addition of LDHs resulted in improved membrane surface hydrophilicity, thereby enhancing water flux. The optimized TFN membrane (0.050 wt% LDH in PIP solution) significantly improved pure water flux, exceeding 150%. All TFN membranes exhibited excellent performance in dye and salt fractionation (93% for Congo red, 2.6% for NaCl, and 40.7% for Na2SO4). Also, excellent self-cleaning ability was observed for the optimized membrane, exhibiting a remarkable water flux recovery rate after three operation cycles. Moreover, including CeZnFe LDH in the optimized TFN membrane played a significant role in enhancing membrane integrity. This study provides new inspiration for fabricating self-cleaning loose NF membranes using CeZnFe LDH for effective dye/salt separation.