The rational use of environmental regulation tools has become an important means by which to improve the efficiency of carbon emissions. Different types of environmental regulations and their combinations have different impacts on carbon emission efficiency. In order to determine the environmental regulation configurations that may achieve high carbon emission efficiency or lead to low carbon emission efficiency, we constructed an analytical framework of connections between environmental regulation configurations and carbon emission efficiency. Moreover, 30 Chinese provinces from the period covering 2016 to 2019 were selected as research cases. In addition, the super slacks-based measure of efficiency (SE-SBM) model was applied to evaluate carbon emission efficiency. Finally, the fuzzy-set qualitative comparative analysis (fsQCA) method was employed to analyze the impact of different environmental regulation configurations on carbon emission efficiency. The results showed that the carbon emission efficiency of various regions of China is generally low (with most regions not having reached an effective level) and that there are large regional differences. We found that there are four environmental regulation configurations that can achieve high carbon emission efficiency and two environmental regulation configurations that lead to low carbon emission efficiency. Based on these configurations, we draw three conclusions: (1) There are three paths to achieving high carbon emission efficiency: one that values command-and-control environmental regulation but disfavors market-incentive environmental regulation, another that combines command-and-control environmental regulation with market-incentive environmental regulation, and a third that couples command-and-control environmental regulation with voluntary environmental regulation. (2) Two paths that may lead to low carbon emission efficiency were established: excessive penalties and the lack of specific measures. (3) In some conditions, environmental governance investment and fiscal expenditure could be substituted for each other; environmental protection administrative penalties and pollution charges are synchronized; environmental governance investment in the promotion of carbon emission efficiency is indispensable. Policies and suggestions on how the government can use environmental regulation tools to improve carbon emission efficiency are proposed from a general coordinative perspective in the final section of this paper.