Grain production (GP) is inherently dependent on ecosystem services (ESs). However, the increasing grain demand heightens the conflict between ESs and GP. This tension is further fueled by unstable natural, socio-economic, and political factors. To reconcile this issue and promote their mutual growth, quantifying the extent to which ESs support GP is essential. This study is designed to present a scientific method for measuring the impact of ESs on GP, thereby enhancing the objectivity and scientific rigor of strategies for ecological and food security. This study, by deconstructing the functional relationship between ESs and GP, employs the Super-SBM model to analyze the mathematical relationships between them, thereby achieving the quantification of the efficiency of ESs in supporting GP. The findings reveal the following key points: (1) the Super-SBM model offers a viable and scientifically robust approach for quantifying the supporting efficiency of ESs on GP; (2) the supporting efficiency of ESs for GP in 93.94% of the counties in the Hengduan Mountainous Region (HMR) is less than 1, indicating that both the efficiency and capacity of regional ESs to support GP are relatively low; (3) an obvious spatial mismatch in allocation is evident between the provision of ESs and the demands of GP in the HMR, which leading to regional supply-demand imbalance; (4) the slack relationships and quantity between ESs and grain output assessed by the Super-SBM model provide a scientific basis and optimization direction for crafting sustainable development strategies between ESs and GP. Supporting efficiency research, as an exploration of the relationship between ESs and GP in the quantitative dimension, represents a deepening of qualitative research, it serves to enhance the scientific basis for sustainable development decisions in the ecological environment and agricultural production, holding a certain degree of positive significance.