In order to address water shortage issues around the world, the collection of fog has been considered as one possible effective solution. In this study, after cultivating several fungi, an abundance of water droplets was found on their surfaces. Based on the morphology and property analyses, a structure that facilitates the effective collection of water was proposed. The structure consists of heterogeneous fiber diameters and a hierarchical structure that provides both hydrophobic and hydrophilic properties. In order to mimic the fungi that collect water, the composite water-collection material was fabricated using a hydrophobic, hierarchical-structured, polyurethane (PU), nanofiber membrane, and hydrophilic filter paper, adhered by polyacrylamide (PAM). The surface of the hydrophilic filter paper captures water droplets from the air, and after the droplets coalesce, the convex structure of the PU membrane allows the membrane to transport the collected water. The water-collection experiment demonstrated that the hydrophilic−hydrophobic amphiphilic materials with thick and thin fibers coexist, and as a result, they can collect water effectively. The water-collection efficiency of the fungi-bioinspired materials achieved a rate of 1018.6 mg cm −2 h −1 when the surroundings were 22 ± 2 °C and 65 ± 5% RH. This work provides a new inspiration and effective methods for the development of bioinspired water-collection materials aimed at solving water shortages.