Ensuring food security and curbing agricultural carbon emissions are both global policy goals. The evaluation of the relationship between grain production and agricultural carbon emissions is important for carbon emission reduction policymaking. This paper took Heilongjiang province, the largest grain-producing province in China, as a case study, estimated its grain production-induced carbon emissions, and examined the nexus between grain production and agricultural carbon emissions from 2000 to 2018, using decoupling and decomposition analyses. The results of decoupling analysis showed that weak decoupling occurred for half of the study period; however, the decoupling state and coupling state occurred alternately, and there was no definite evolving path from coupling to decoupling. Using the log mean Divisia index (LMDI) method, we decomposed the changes in agricultural carbon emissions into four factors: agricultural economy, agricultural carbon emission intensity, agricultural structure, and agricultural labor force effects. The results showed that the agricultural economic effect was the most significant driving factor for increasing agricultural carbon emissions, while the agricultural carbon emission intensity effect played a key inhibiting role. Further integrating decoupling analysis with decomposition analysis, we found that a low-carbon grain production mode began to take shape in Heilongjiang province after 2008, and the existing environmental policies had strong timeliness and weak persistence, probably due to the lack of long-term incentives for farmers. Finally, we suggested that formulating environmental policy should encourage farmers to adopt environmentally friendly production modes and technologies through taxation, subsidies, and other economic means to achieve low-carbon agricultural goals in China.