Membrane separation technology has emerged as a powerful tool to separate organic dyes from industrial wastewater. However, continuously selective separation of organic dyes with similar molecular weight remains challenging. Herein, we presented a pH-triggered membrane composed of polydopamine-decorated tunicate-derived cellulose nanofibers (PDA@TCNFs) for selective separation of organic dyes. Such self-supporting membranes with nanoporous structure were fabricated by facile vacuum-assisted filtration of PDA@TCNF suspension. The incorporation of polydopamine not only enhanced the stability of the membranes, but also endowed membranes with excellent pH sensitivity, facilitating the continuously selective separation of organic dyes. These pH-triggered PDA@TCNF membranes could selectively separate Methyl Orange (MO) and Rhodamine B (RB) from the MO/RB mixed solution by switching the pH values. The continuously selective separation of the MO/RB mixed solution was demonstrated, where both MO and RB recovery ratios maintained at ∼99 % during 50 repeated cycles. This work provides a new strategy to develop a pH-triggered sustainable nanocellulose-based membrane for continuously selective separation of mixed dyes.