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This paper presents a modelling approach to the design optimization of Selective Catalytic Reduction (SCR) systems. The present study is concerned with ammonia slip and conversion efficiency of oxides of nitrogen (NOx), which are two major issues of SCR technologies. A Computational Fluid Dynamics (CFD) code is employed to simulate the mixing characteristics with the purpose of optimization of the concentration distribution of the reducing agent. The physical processes including urea spray atomization, droplet evaporation, urea decomposition and turbulent mixing are accounted for in the modelling method. The Lagrangian discrete phase model is used to describe the urea spray, which contains sub-models for droplet breakup and evaporation. A reaction model of urea decomposition is proposed. The geometry of a specific example includes two air-assisted fluid nozzles, optimized mixing elements of the static mixer, and the SCR converter with two layers of substrates.