The Chinese government adheres to the innovation driven strategy and emphasizes that technological innovation is the strategic support for improving social productivity and comprehensive national strength. This paper discusses the mechanism of technological innovation and regional economic co-evolution, and constructs an index system to assess them based on the principles of synergy and systematics. The authors use a dynamic coupling model to study the law of the cooperative evolution of composite systems and geo-detector methods to reveal the main factors controlling the degree of coordination among them. The results show that the total factor productivity of China's high-tech industry showed a "W"-type trend of change from 2006 to 2016, and the other indices exhibited a volatile trend. The total factor productivity, technical efficiency, scale efficiency, pure technical efficiency, and technological progress increased by 37%, 13.3%, 3.9%, 9%, and 20.8%, respectively. There was a significant spatial difference in changes in total factor productivity, forming a core-edge spatial pattern with the middle and upper reaches of the Yangtze River as the center of concentration. Most of China's technological innovation and regional economic complex systems were in a state of interactive development from 2007 to 2016, except in the three northeastern provinces of Zhejiang, Shanghai, and the western part of the country. The degree of coupling of the other provinces showed an increasing trend, and the overall degree of coupling exhibited the spatial pattern of Central > Eastern > Western > Northeastern. The three most influential factors for the degree of coupling of China's provincial complex system were the gross domestic product, efficiency of technological innovation, and expenditure on research and development, whereas the three most important factors affecting the degree of coupling of complex systems were the efficiency of technological innovation, gross domestic product, and number of high-tech enterprises as well as research and development personnel, respectively, in the eastern, central, western, and northeastern regions. Finally, the paper puts forward the suggestions of regional innovation driven coordinated development, technology innovation and regional economic coordinated development, in order to provide reference for the high-quality economic development of developing countries.