An efficient method of coating alumina (Al2O3) on stainless steel has been investigated by matching the rough surface of the substrate with different sizes of Al2O3 particles. An empirical correlation was established based upon the data of a controllable and measured pore size of the substrate surface by varying etching conditions. The correlation agreed fairly well with experimental results (deviations of +/- 20%). The Al2O3 coatings prepared by powders with average particle size of 324 nm had an optimal adhesion performance, and the minimum of coating weight loss on the inner surface of tubule after ultrasonic vibration was 1.7 wt %. The developed method of Al2O3 coating has potential prospects for the preparation of monolithic catalyst support.