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In the logarithmic curves of the per capita GDP and the urbanization, with the traditional environmental Kuznets equation, this paper presented a coupling equation showing the relationship between urbanization and the atmospheric environment. Based on the 'double exponential' coupling curve, the principles of flattening, advancing and fast-falling that new coupling curve should be followed were discussed. According to the two indicators of environmental assessment, namely the treatment cost and the deterioration degree of the environment, a new dual four times matrix model with the corresponding countermeasures and environment policy were introduced. Taking Shandong Province as an example, the coupling relationship between urbanization and atmospheric environment was investigated. The coupling curve showed that it was in running-in stage, and atmospheric quality tended to be improved. SO curve fluctuated more significantly compared with soot and industrial dust curves. The matrix model shows that the combination of flattening principle and advancing principle is preferable for SO emissions, but the fast-falling principle is recommended for soot and industrial dust emissions. [ABSTRACT FROM AUTHOR]