Utilizing membrane separation technology has displayed promising application potential for removing synthetic dyes; however, membrane performance tends to decline over time due to fouling caused by feed solution contaminants, leading to decreased separation efficiency and shortened membrane lifespan. Therefore, improving the antifouling properties of membranes is critical to ensure the long-term efficiency of water treatment systems. In this work, a high-performance catalyst, CuZn@ZC, with remarkable oxygen activation activity, was successfully prepared and subsequently integrated onto the membrane surface via simple pumping filtration, resulting in self-cleaning membranes with superior antifouling capabilities. The results indicated that zero-valence copper containing CuZn@ZC can rapidly and efficiently remove a wide range of dyes under mild natural conditions, accompanied by strong 1O2 and •O2– signals detected in electron paramagnetic resonance spectra. When applied to membrane surfaces, the modified membrane exhibited excellent antifouling and filtration properties, which showed high flux recovery ratios and a superior rejection rate for cationic dyes, attributed to the participation of ROS generated by the activation of natural dissolved oxygen. Moreover, the membrane still retained its structural stability and environmental compatibility during prolonged operation, which is beneficial for advancing the development of sustainable membrane filtration technologies.