Various ordered nanoporous alumina films with arbitrary pore intervals from 130 to 980 nm were fabricated on aluminum by a critical-potential anodization approach with sulfuric, phosphoric, oxalic, glycolic, tartaric, malic, and citric acid electrolytes under 70-450 V. The pore intervals of the porous alumina films were linearly proportional to applied potentials, with corresponding dominated territories to the electrolytes. In addition to pore interval, the self-ordering extent of pore arrangement was also improved with increasing anodizing potentials, leading to highly ordered porous alumina films at critical-high potentials. A cell separation phenomenon occurred for the films formed in sulfuric and glycolic acid solutions at the critical potentials, thus leading to the formation of highly ordered alumina nanotubule arrays. The critical-potential anodization in the other electrolytes produced self-organized porous alumina films with two-layered pore walls and pore bases. The basic principle for achieving porous alumina films with desired pore intervals is controlling the balance of the growth of barrier layer and the pore generation by adjusting the acidity, the concentration, and temperature of electrolytes. The porous alumina films formed in various electrolytes were transparent, and the transmittances of the films were inversely proportional to the applied potentials or the pore intervals. (c) 2006 The Electrochemical Society.