In order to explore and optimize the internal connection and coupling coordination path between technological innovation in high-tech industry and high-quality development of regional economy, and the benign interaction and coordinated development between them were promoted. From the perspective of eight comprehensive economic zones, the coupling coordination degree and relative development degree models were used to measure the coupling and coordination state and relative development degree of the technological innovation in the high-tech industry and the high-quality development of regional economy from 2010 to 2020, and its spatial correlation was tested, and the key obstacle factors were diagnosed with the help of obstacle degree model. The results show that the relative difference between the technological innovation in the high-tech industry and the high-quality development of the regional economy was obvious in the comprehensive economic zones from 2010 to 2020, and the Northern coastal, Eastern coastal, and Southern coastal economic regions were much higher than the Northwest economic regions. The degree of coupling and coordination between the technological innovation in the high-tech industry and the high-quality development of the regional economy was different in the eight comprehensive economic zones from 2010 to 2020, and the Eastern coastal economic region had reached a high level of coupling and coordination, while the Mid-Yangtze River had a benign coupling and a low level of coordination. The speed of technological innovation in high-tech industry lagged and restricted the high-quality development of the regional economy in the Mid-Yangtze River, the Mid-Yellow River, the Great Southwest, and the Great Northwest economic regions, while the Southern Coastal region was in a state of synchronous development. The key obstacle factors of the elements layer and the indexes layer were different in each integrated economic zone, but it reflected the main obstacle of the coordinated evolution of the coupled system.