This paper uses panel data from 30 provinces and cities in China between 2008 and 2017. It calculates the green innovation performance of each province and city based on the super-efficiency SBM model of unexpected output and measures the high-tech industrial agglomeration degree of each province and city by using the location entropy method. The influence of high-tech industrial agglomeration on green innovation is also empirically tested. It is found that the agglomeration level of high-tech industry and green innovation performance in Eastern China are much higher than those in Central and Western regions. There is a significant positive relationship between high-tech industrial agglomeration and green innovation performance. Human capital has a mediating effect in the positive impact of high-tech industry agglomeration on green innovation performance. The moderating effect of environmental regulation is markedly established. The higher the level of environmental regulation, the stronger the mediating effect of human capital. Based on the above conclusions, this paper puts forward relevant policy suggestions for promoting the organic combination of green and innovation-driven development and for promoting green transformation in China.