The role of spatial factors in reducing carbon emissions has been receiving increasing attention from researchers; however, these impacts may involve spatial heterogeneity. In this study, 337 prefecture-level cities in China were taken as the research object. Based on national-level urban data, the global impact of urban spatial form on carbon emissions was then investigated using ordinary least squares regression, the spatial error model, and the spatial lag model. The local effects of urban spatial form on carbon emissions in different cities were then investigated using geographically weighted regression. The findings are as follows. Overall, the larger the urban built-up area and the more fragmented and decentralized the urban land use, the greater the carbon emissions. Conversely, the more centralized the urban center of a city, the lower its carbon emissions. Locally, for some Chinese cities, the total area, landscape shape index, and mean Euclidean nearest-neighbor distance were found to have significant positive effects on carbon emissions, while the largest-patch index had a significant negative impact. For all Chinese cities, the patch density was found to have no significant effect on carbon emissions. In 29% of the cities in which the landscape division index was found to significantly affect carbon emissions, this effect was positive, while it was negative in the remaining 71%. The policy implications emerging from this study lie in the need for decision-makers and urban planners to guide the shaping of low-carbon urban spatial forms.