The technological innovation and high-tech industrial agglomeration are important parts of regional economic growth process, and also the inevitable path to optimize the resources and upgrade the industrial structure. The paper selects the perspective of regional technical innovation efficiency to study the interaction between the high-tech industrial agglomeration and the technological innovation, which have significant meaning for the economic transformation and the construction of an innovative country. With “the High-Tech Industrial Agglomeration and the Efficiency of Regional Technological Innovation” as the theme, the paper comb the theories and mechanism analysis of the high-tech industrial agglomeration and the technological innovation. On this basis, this paper measures the high-tech industrial cluster and regional characteristics of Chinese mainland, and estimates the overall efficiency and the two-stage efficiency of regional technical innovation. Then this paper studies how the industrial agglomeration affects the regional innovation efficiency and how the regional innovation efficiency affects the industrial agglomeration from the theoretical and empirical perspective. The measurement results show that, both have serious spatial imbalance phenomenon, but also show the strong regional convergence. We discover the mutual promotion and mutual adaptation relationship of the high-tech industrial agglomeration and the technological innovation, each other having a significant positive. The results show that, the diversification has a significant positive effect to the regional technological innovation efficiency, and the technology transfer efficiency performs a more significant role for the high-tech industrial agglomeration. Moreover the interaction is also affected by a series of constraints. We should promote the high-tech industry agglomeration reasonably, enhance the regional technology innovation efficiency, improve “industry-university-government” innovative functions, bring the link boost function of financial market into full play, strengthen college scientific and technological achievements conversion, so that to promote coordinated development of technological innovation efficiency and high-tech industrial agglomeration and to promote regional economic growth and industrial restructuring.