Abstract: Promoting the green and low-carbon transformation of agriculture and strengthening the national food security barrier are urgent requirements for China to practice ecological civilization construction and achieve high-quality agricultural development in the new era. The “Chinese path to modernization” pursues harmonious coexistence between humans and nature, requiring agricultural development to balance the bottom line of food security with the goals of green and low-carbon development, fostering their positive synergistic growth. Based on provincial panel data from 2013 to 2022 and grounded in the diversified food supply perspective, this study explored the coupling coordination and spatiotemporal evolution of food security and agricultural green and low-carbon development under the background of the grand food perspective. The findings revealed that from 2013 to 2022, both food security levels and agricultural green and low-carbon development levels in China had exhibited an upward trend, with the former experiencing a greater increase and the latter remaining relatively high overall. The growth of both factors converged over time, with coordination levels gradually improving but significant regional disparities persisting. Spatially, the pattern exhibited as “stronger in the east and weaker in the west, higher in the north and lower in the south”, showing significant agglomeration but weakening directional spatial differences. Therefore, it is recommended to address imbalances by category, establish a pattern of “east-west linkage and north-south coordination”, and reduce regional disparities.