During the “14th Five-Year Plan” period, a question worth exploring in depth would be how China promotes green development through green finance to realize the goal of financially supporting the construction of ecological civilization. This paper builds a super-efficiency SBM window model to evaluate the comparable eco-efficiency of 30 provincial administrative regions in Mainland China (except Tibet) as a measurement of green development, and constructs an evaluation system for the green finance index, as a measurement of regional green finance development levels in China from 2007 to 2019. This paper also constructs spatial econometric models to study the effects of green finance on green development, and the influence of green finance on green development through supporting green technological innovation. Moreover, this paper analyzes the mechanisms of the spatial spillover effects and the heterogeneity in eastern, central, and western regions of China. The results of the study show that green finance only has a positive effect on green development in eastern regions, while in central and western regions, it fails to effectively support green development. The positive effect of green finance on green development by supporting green technological innovation is only in eastern regions, but it is not significant in the central region, while negative effect in the western region. Finally, according to the research conclusions, it is proposed to implement differentiated policies of green finance and the integration policies of green finance and green technological innovation policies in different regions of China.