Food, water, carbon, and land are pivotal for achieving the SDGs. Focusing on the Chinese Loess Plateau (2000-2020), we quantify ecosystem service supply, demand, and their balance with food production, water yield, carbon storage, and the sediment delivery ratio, and examine spatiotemporal patterns, ecosystem service bundles and drivers. Supply rose by 82.60% (food production), 44.50% (water yield), 1.70% (carbon storage), and 37.20% (sediment delivery ratio), with a southeast-high, northwest-low gradient. Demand fell about 30% for food production and water yield but increased by 166.60% and 8.50% for carbon storage and sediment delivery ratio. Cropland percentage, forestland coverage, built-up land percentage, precipitation, elevation, and GDP per unit area were dominant drivers with strong spatial heterogeneity. Spatially, water yield and carbon storage ratios were most deficient in highly urbanized areas, whereas food production and sediment delivery ratio were higher in forested zones. Based on these patterns, this paper delineates a grain-ecology coordination zone, a grain production core area, and an ecological restoration area, and proposes targeted strategies to advance SDG-aligned regional sustainability. The study enriches the understanding of ecosystem service supply and demand relationships and supports grain ecological security on the Chinese Loess Plateau and other similar regions.