Copper is a major problem in industrial wastewater streams, seriously affecting the quality of potential drinking water. Several approaches, including continuous membrane processes or batch-wise application of adsorbents, are in use to tackle this problem. Unfortunately, these processes suffer from their particular drawbacks, such as low permeance or disposal of saturated adsorbents. However, a combination of these processes could constitute a step towards a more efficient copper removal solution. Here, we present a nanopaper ion-exchanger prepared from cellulose nanofibrils produced from fibre sludge, a paper industry waste stream, for the efficient, continuous removal of copper from aqueous solutions. This nanopaper ion-exchanger comprises phosphorylated cellulose nanofibrils that were processed into nanopapers by papermaking. The performance of these phosphorylated nanopaper membranes was determined with respect to their rejection of copper and permeance. It was shown that this new type of nanopaper is capable of rejecting copper ions during a filtration process by adsorption. Results suggest that functional groups on the surface of the nanopapers contribute to the adsorption of copper ions to a greater extent than phosphate groups within the bulk of the nanopaper. Moreover, we demonstrated that those nanopaper ion-exchangers could be regenerated and reused and that in the presence of calcium ions, the adsorption capacity for copper was only slightly reduced.