This paper presents a model-aided approach to the development of catalysts for CO oxidation. This is in contrast to the traditional methodology whereby experiments are guided based on experience and intuition of chemists. The proposed approach operates in two stages. To screen a promising combination of active phase, promoter and support material, a powerful "space-filling" experimental design (specifically, Hammersley sequence sampling) was adopted. The screening stage identified Au-ZnO/Al(2)O(3) as a promising recipe for further optimization. In the second stage, the loadings of Au and ZnO were adjusted to optimize the conversion of CO through the integration of a Gaussian process regression (GPR) model and the technique of maximizing expected improvement. Considering that Au constitutes the main cost of the catalyst, we further attempted to reduce the loading of Au with the aid of GPR, while keeping the low-temperature conversion to a high level. Finally we obtained 2.3% Au-5.0%ZnO/Al(2)O(3) with 21 experiments. Infrared reflection absorption spectroscopy and hydrogen temperature-programmed reduction confirmed that ZnO significantly promotes the catalytic activity of Au. (C) 2011 Elsevier B.V. All rights reserved.