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A simple and economical approach to the preparation of superhydrophilic and water-capturing surfaces is reported. In this method, a common polymer aqueous blend is drop-cast onto a substrate, and the natural drying of the aqueous drop allows for the formation of phase-segregated nanosegregants between the bulk film and substrate surface. The nanosegregant is then exposed by dissolving the bulk film using water. The nanosegregant is stable, water-insoluble and optically transparent, and exhibits superhydrophilicity with a minimum contact angle below 10 degrees. It also displays strong water-attracting ability. The mechanism of superwettability and water-capturing behavior is discussed in terms of the self-organization and functional group of the nanosegregant.