A novel superhydrophilic material, charged polymer brushes-grafted magnetic core-shell-corona composite nanoparticles (Fe3O4@SiO2@PSPMA), was developed to harvest water through the hydration effect. Because of both the strong hydration capability and the good swelling performance, the negatively charged polymer brushes, PSPMA brushes, endow the composite nanoparticles with superhydrophilicity and a good water-absorbing performance like a sponge, while the magnetic Fe3O4 cores allow easy separation of Fe3O4@SiO2@PSPMA nanoparticles with absorbed water from oil/water mixture under an external magnetic field. The functional particles have the capability of harvesting water droplets whether floating on an oil surface or in the oil. This water-absorbing material uses selective wettability to harvest water and achieve oil-water separation and may be useful in finding novel approaches for recycling water from sewage and removing water in the petroleum industry.