A straightforward approach was successfully developed to fabricate a well-designed three-dimensional rough sheetlike MgAl-layered double hydroxide (LDH) array to stand vertically on poly(acrylonitrile) porous nanofibrous membranes based on an electrospun-nanofiber-templated in situ hydrothermal strategy, and then the surface was modified with cyclohexanecarboxylic acid. The as-spun highly dense ordered sheetlike LDH porous nanofabric exhibited a superior durability in superhydrophobicity and superoleophilicity, which has achieved high oil-removing capability including both oil harvesting and oil separation to harvest/separate a wide range of organic solvents and oils from an oil water mixture and, especially, exhibited a very good recycling and reusing performance. Interestingly, a steady water repellency was obtained against both drinkable hot (about 95 degrees C) and cool water. Outstanding oil harvesting, oil separation, and highly durable water repellant can be attributed to an effective synergistic effect between the high-density roughness of LDH nanosheets modified with acid and the very high porosity in the electrospun nanofibers, as well as the interspace between LDH nanosheets that acted as both a textile for selective oil separation and a container for penetrated oil storage, leading to special wettability, making the as-spun nanofabric a promising textile for large-scale removal and recollection of hydrophobic spillage on the water surface.