Well-defined and uniform pore-structure (WDUPS) Al2O3 catalyst supports were prepared by coating specially treated SiO2 opals with Al2O3. The pore-size of the WDUPS Al2O3 can be tailored in the range of meso- to macro-size by using different-sized microspheres to fabricate the SiO2 opal. The optimal amount of Al2O3 coating, which keeps the pore structure of SiO2 template intact, was determined to be of the 1-2 atomic layers. The surface acid amount of WDUPS Al2O3 significantly increased with the Al2O3 coating until one atomic layer formed. When the SiO2 opals were coated with optimal amount of Al2O3, the obtained WDUPS Al2O3 showed a uniform acid density. With these characteristics, the WDUPS Al2O3 support is ideal material for fundamental research in catalysis. The method is promising strategy to obtain other catalytic materials with the same structure. (C) 2013 Elsevier B.V. All rights reserved.