Constructing CuO-based nanofibrous membranes with remarkable mechanical performance, controllable nanostructures, and outstanding catalytic oxidation activity would be conducive to decomposing organic contaminants in wastewater through advanced oxidation processes; however, there remains a huge shortfall of such ceramic membranes that they are usually fragile with poor deformability. Herein, a universal approach was proposed for fabricating flexible CuO nanoparticles-anchored ZrO2 nanofibrous membranes (CZNMs), that is, through the combination of successive ionic layer adsorption and reaction (SILAR) assembly and the follow-up thermal oxidation processes. Notably, the developed preparation method exhibited strong expansibility, which could be extended to the synthesis of other flexible metal oxides/ceramic nanofibrous composites, such as ZnO/ZrO2, CdO/ZrO2, and Mn3O4/ZrO2. Profiting from the integrated advantages of superior catalytic reactivity, uniform nanostructures distribution, and excellent mechanical properties, the resultant CZNMs displayed a prominent degradation efficiency of 92.4% within 50 min towards tetracycline hydrochloride under the activation of peroxymonosulfate (PMS). Furthermore, the stable hierarchical structures and robust mechanical performance endow the as-synthesized membranes with extraordinary reusability and easy recycling. The successful preparation of such ceramic-based nanofibrous membranes with superior flexibility and high-efficient catalytic performance might provide some reference to develop other synergetic membranous catalysts for wastewater treatment.