Based on the development philosophy of “innovation, coordination, green, open, sharing”, a high-quality development index system is built to evaluate and measure the regional high-quality development level with the entropy method, and to analyze the convergence status and convergence mechanism of regional high-quality development. In order to further clarify the driving factors of high-quality development, a coupling model is used to analyze the degree of coordinated development between regional innovation capabilities and high-quality development levels, a conditional convergence model is employed to test the innovation mechanism of high-quality development. The result shows that China’s regional high-quality development level has been steadily improved from 2000 to 2017, however, there is a ladder-like regional difference of “high in the east and low in the west”. Except for northeast China, there is a trend of convergence from regions with low level of high-quality development to regions with high level, with constraint conditions on convergence. From 2000 to 2017, China’s innovation capability and the degree of coordination between it with high-quality development have been steadily improved, but the driving effect of innovation in different regions is heterogeneous.