Most of the world's grasslands are managed for livestock production. A critical component of the long-term sustainability and profitability of rangelands (e.g., grazed grassland ecosystems) is the maintenance of plant production. Amending grassland soils with organic waste has been proposed as a means to increase net primary productivity (NPP) and ecosystem carbon (C) storage, while mitigating greenhouse gas emissions from waste management. Few studies have evaluated the effects of amendments on the C balance and greenhouse gas dynamics of grasslands. We used field manipulations replicated within and across two rangelands (a valley grassland and a coastal grassland) to determine the effects of a single application of composted green waste amendments on NPP and greenhouse gas emissions over three years. Amendments elevated total soil respiration by 18% ± 4% at both sites but had no effect on nitrous oxide or methane emissions. Carbon losses were significantly offset by greater and sustained plant production. Amendments stimulated both above- and belowground NPP by 2.1 ± 0.8 Mg C/ha to 4.7 ± 0.7 Mg C/ha (mean ± SE) over the three-year study period. Net ecosystem C storage increased by 25–70% without including the direct addition of compost C. The estimated magnitude of net ecosystem C storage was sensitive to estimates of heterotrophic soil respiration but was greater than controls in five out of six fields that received amendments. The sixth plot was the only one that exhibited lower soil moisture than the control, suggesting an important role of water limitation in these seasonally dry ecosystems. Treatment effects persisted over the course of the study, which were likely derived from increased water-holding capacity in most plots, and slow-release fertilization from compost decomposition. We conclude that a single application of composted organic matter can significantly increase grassland C storage, and that effects of a single application are likely to carry over in time.