Green infrastructure (GI) plays a pivotal role in contemporary urban infrastructure. Green infrastructure investment (GII) provides a fresh perspective for controlling urban carbon emissions in the context of global climate change. Based on theoretical analysis, we employed panel data from Chinese cities to examine the effects and operating mechanisms of GII on urban carbon emissions. The research reveals that the incremental GII can notably decrease urban carbon emissions, and various robustness tests and endogeneity checks corroborate this finding. However, when considering the cumulative effect, the GII stocks do not appear to influence urban carbon emissions; GII mitigates urban carbon emissions by drawing in pollution control talents, improving the efficiency of household waste treatment, increasing urban green spaces, and heightening public attention to the environment. Relative to cities in the central-western region, northern cities, smaller cities, resource-based cities, smart pilot cities, and cities with a lesser environmental emphasis, GII is more effective in curbing carbon emissions in eastern cities, southern cities, larger cities, non-resource-intensive cities, cities not in the smart pilot initiative, and cities with a stronger environmental focus. This research enhances the understanding of GI’s environmental outcomes and the determinants of urban carbon emissions from an investment viewpoint. It also dissects the four operative mechanisms through which GII lowers urban carbon emissions, offering a novel interpretation of GII for the variance in carbon emission levels across cities with diverse traits.