Maintaining crop outputs to feed its large population with limited resources while simultaneously mitigating carbon emissions are great challenges for China. Improving the efficiency of resource use in crop production is important in reducing carbon emissions. This paper constructs a methodological framework combining emergy-based indicator accounting and a nonseparable undesirable output slack-based measurement (SBM) data envelopment analysis (DEA) model. This framework is used to explore the efficiency of inputs and outputs and the greenhouse gas (GHG) emissions reduction potential for crop production systems, using Zhejiang province, China, as a case study. It is found that an emergy synthesis and a nonseparable undesirable output SBM-DEA framework is compatible with the case study. Crop production in Zhejiang province has relied heavily on an increase in agrochemical inputs to maintain agricultural output. Energy and chemical fertilizer use are determined as the province's major carbon emissions sources. Although carbon emissions per unit of monetary output has decreased sharply, the carbon emissions per unit emergy output has increased, demonstrating a high carbon intensity reality. The DEA highlighted the differences in crop production efficiency, resource factor redundancy and carbon mitigation potential in the different prefectures of the province. To conclude this research, policies to support low carbon agriculture development, including subsidizing low carbon agriculture technology development and expansion and the cancellation of subsidies to high carbon production factors, such as chemical fertilizer production and sales, are discussed to conclude the research.