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Because of the complex and special political relationship between Mainland China and Taiwan. Cross-Strait trade is influenced by many variables, there has been a view that trade relations between Mainland China and Taiwan are more influenced by political factors. However, between the Cross-Strait, the trade volume has generally shown an upward development trend, especially since 2001. Therefore, the political factors can hardly explain the facts, and economic factors, especially industrial structure factors in Mainland China play an important role in Cross-Strait trade. Based on the small sample data since 2001, this study employed Grey Relational Analysis （GRA） method to verify the evolution of Mainland China's industrial structure and Cross-Strait trade. Based on the results show that the evolution of Mainland China's industrial structure strongly impacts the development of Cross-Strait trade. The tertiary industry has the strongest correlation with Cross-Strait trade, followed by the secondary and primary industries. Furthermore, the evolution of the mainland's industrial structure will expand as well as accelerate the imbalance of Cross-Strait trade. [ABSTRACT FROM AUTHOR]