Only through successful transformation and application in industries, technology achievements in universities can promote economic and social development. Meanwhile, technological progress in high-tech industries depends in part on universities’ technology achievements. Coupling coordination between technology transfer in universities (TTU) and high-tech industries development (HTID) is of great significance to the sustainable development of the regional sci-tech innovation system. In this paper, the coupling mechanism of TTU and HTID is analyzed and comprehensive evaluation index systems are established by using the evaluation indicator to screen and assign weights based on information contribution rate. The coupling coordination index (CCI) and productivity index (PI) are introduced to derive the spatiotemporal characteristics of the coupling and coordination of TTU and HTID from 2010 to 2019 in China and analyze its influence factors by System-Generalized Method of Moments (SYS-GMM). The results show the following: (1) the overall national TTU-HTID CCI shows a gradual upward trend and large regional differences; (2) CCI of most provinces is increasing, but the differences are widening; (3) the national TTU PI is in a state of volatility and decline, but the ability of TTU is still much higher than the level of HTID; (4) technological innovation in high-tech industries, high-tech industry technology absorption capacity, high-tech industry development level, industry-university cooperation, and technological finance development have significant roles in promoting the coupling coordination of TTU-HTID. Meanwhile, the sci-tech innovation level in universities, technology transferability in universities, government support, development of sci-tech intermediary, and development of other research institutions have no significant impact.