We report a facile nanofabrication method, one-step hard anodizing and etching peeling (OS-HA-EP) of aluminum foils followed by multistep mild anodizing and etching pore-widening (MS-MA-EW), for the controllable tailoring of hexagonally packed three-dimensional alumina taper-nanopores. Their profiles can be precisely tailored by the synergistic control of anodizing time, etching time and cyclic times at the MS-MA-EW stage, exemplified by linear cones, whorl-embedded cones, funnels, pencils, parabolas, and trumpets. Meantime, their periods can also be modulated in the range of 70–370 nm by choosing matched anodizing electrolytes (e.g., H₂C₂O₄, H₂SO₄, H₂C₂O₄–H₂SO₄, and H₂C₂O₄–C₂H₅OH mixture) and anodizing voltages at the OS-HA-EP stage. We also demonstrated that the long-range ordering of nanopits and the peak voltage of stable self-ordered HA, which are unachievable in a single H₂C₂O₄ electrolyte system, can be effectively tuned by simply adding tiny quantity of H₂SO₄ and C₂H₅OH to keep an appropriate HA current density, respectively. This method of using the combination of simple pure chemical nanofabrication technologies is very facile and efficient in realizing the controllable tailoring of large-area alumina membranes containing self-ordered taper-nanopores. Our work opens a door for exploring the novel physical and chemical properties of different materials of nanotaper arrays.