Virus removal can be successfully achieved based on an electrostatic adsorption mechanism. The key requirement for this process is to develop filter materials that can be produced by low-cost technologies and are suitable in large-scale production for real applications. In this study, we report development of spray-dried alumina granules modified with copper (oxide) nanoparticles and critically assess the effect of copper oxidation state on virus removal capacity. Using plate-shaped alumina as a support material resulted in porous structure, which in turn ensured prolonged contact time of contaminated water with the material. Subsequently, copper (oxide) nanoparticles provided a large number of adsorption sites. Flow experiments revealed that copper(I) oxide and metallic copper were the active phases in virus removal and 99.9% of MS2 bacteriophages could be removed. However, almost no virus removal was observed in the presence of copper(II) oxide. Contrasting virus removal characteristics are associated with the different surface charge of copper species, as determined by zeta potential measurements.