Over recent decades, both global cropland areas and synthetic nitrogen (N) fertilizer application have greatly increased to feed the growing population (FAOSTAT, 2023) but with large detrimental side-effects on the environment. Estimates suggest that the conversion of natural vegetation (e.g., forests and grasslands) to cropland has reduced soil organic carbon (SOC) stocks by 32%-36% in temperate (Poeplau et al., 2011) and 25%-30% in tropical regions (Don et al., 2011). Management intensification has also caused soil fertility decline (Lal, 2004), air pollution (Reay et al., 2012;Tian et al., 2020), and freshwater eutrophication (Moss, 2008). Gaseous N emissions from fertilizer application have increased by 46% (to 3.8 Tg N yr −1 ) for nitrous oxide (N 2 O) (Tian et al., 2020) and by 78% (to 58 Tg N yr −1 ) for ammonia (NH 3 ) (L. Liu et al., 2022) over the past four decades. The SOC loss from the expansion and management of agricultural land, combined with the N loss from the intense use of Abstract Cover crops (CCs) can improve soil nutrient retention and crop production while providing climate change mitigation co-benefits. However, quantifying these ecosystem services across global agricultural lands remains inadequate. Here, we assess how the use of herbaceous CCs with and without biological nitrogen (N) fixation affects agricultural soil carbon stocks, N leaching, and crop yields, using the dynamic global vegetation model LPJ-GUESS. The model performance is evaluated with observations from worldwide field trials and modeled output further compared against previously published large-scale estimates. LPJ-GUESS broadly captures the enhanced soil carbon, reduced N leaching, and yield changes that are observed in the field. Globally, we found that combining N-fixing CCs with no-tillage technique could potentially increase soil carbon levels by 7% (+0.32 Pg C yr −1 in global croplands) while reducing N leaching loss by 41% (−7.3 Tg N yr −1 ) compared with fallow controls after 36 years of simulation since 2015. This integrated practice is accompanied by a 2% of increase in total crop production (+37 million tonnes yr −1 including wheat, maize, rice, and soybean) in the last decade of the simulation. The identified effects of CCs on crop productivity vary widely among main crop types and N fertilizer applications, with small yield changes found in soybean systems and highly fertilized agricultural soils. Our results demonstrate the possibility of conservation agriculture when targeting long-term environmental sustainability without compromising crop production in global croplands.