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Sensitive detection and effective removal of copper ions (Cu 2+ ) from water are still arduous tasks required to protect public health and environmental safety because of the serious impacts of Cu 2+ on humans and other organisms. Herein, we report the design and fabrication of self-supporting flexible amidated polyacrylonitrile/branched polyethyleneimine nanofiber membranes (abbreviated as aPAN/BPEI NMs) via facile electrospinning and a subsequent hydrothermal method, which are used not only as strips for the visual detection of Cu 2+ but also as effective adsorbents for the removal of Cu 2+ from water. Because aPAN/BPEI NMs are self-supporting, they can be easily removed from the solution to reduce secondary pollution to the environment. Based on the high Cu 2+ binding capacity of BPEI, Cu 2+ ions are adsorbed on the aPAN/BPEI NMs, which leads to the appearance of new absorbance bands at 280 and 636 nm and a color change from yellow to blue. aPAN/BPEI NMs are utilized for the visual detection of Cu 2+ with a linear range of 50−700 μM and limits of detection of 11.5 and 4.8 μM (absorption peaks at 280 and 636 nm). More importantly, aPAN/BPEI NMs exhibit excellent selectivity and certain recovery with a simple treatment. Furthermore, by utilizing the adsorption characteristics of Cu 2+ in aqueous media, it can be effectively removed by aPAN/ BPEI NMs with a remarkable adsorption capacity of 209.53 mg•g −1 . Additionally, the removal of Cu 2+ by aPAN/BPEI NMs does not exhibit interference by other foreign ions. The adsorption process conforms well to the pseudo-second order (PSO) kinetic model and Jovanovich model, proving that adsorption occurs via chemical and monolayer adsorption mechanisms. Accordingly, this work will provide theoretical and technical support for the design and fabrication of novel heavy metal ion detection-removal integrated materials exhibiting high sensitivity and strong adsorption.