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Optimizing the layout of the urban street canyon to achieve the maximum environmental benefits should become a new idea for modern urban street design and planning. This paper aims to find out the optimized street canyon from a viewpoint of environmental protection by using the two-dimensional numerical simulation model with the turbulence model, coupling with the mathematical optimization method. The total pollutant concentration within and at top of the specific street canyons was taken as the objective function, and the height of one side of the canyon as the constrained condition. A nonlinearly improved constrained variable metric solver was used. The effect of the height of the leeward building and windward building on the integrated pollutant dispersion was studied to achieve the most beneficial configuration of the urban geometry. The optimization of layout for an asymmetrical street canyon was obtained. It is further found that the step-down street canyon with a large height difference is generally a good layout favoring to reduce the concentration accumulation in the street canyon.